WO2019121766A1 - Unité de construction pour échangeur de chaleur magnétocalorique - Google Patents

Unité de construction pour échangeur de chaleur magnétocalorique Download PDF

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Publication number
WO2019121766A1
WO2019121766A1 PCT/EP2018/085629 EP2018085629W WO2019121766A1 WO 2019121766 A1 WO2019121766 A1 WO 2019121766A1 EP 2018085629 W EP2018085629 W EP 2018085629W WO 2019121766 A1 WO2019121766 A1 WO 2019121766A1
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WIPO (PCT)
Prior art keywords
substrate
building unit
base plate
shaped body
ridges
Prior art date
Application number
PCT/EP2018/085629
Other languages
English (en)
Inventor
Colman Carroll
Dietmar Bender
Herve Dietsch
Christian Eichholz
Benjamin SCHMIDT-HANSBERG
Original Assignee
Basf Se
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
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Application filed by Basf Se filed Critical Basf Se
Publication of WO2019121766A1 publication Critical patent/WO2019121766A1/fr

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/012—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials adapted for magnetic entropy change by magnetocaloric effect, e.g. used as magnetic refrigerating material
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25B—REFRIGERATION MACHINES, PLANTS OR SYSTEMS; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS
    • F25B21/00—Machines, plants or systems, using electric or magnetic effects
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25B—REFRIGERATION MACHINES, PLANTS OR SYSTEMS; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS
    • F25B2321/00—Details of machines, plants or systems, using electric or magnetic effects
    • F25B2321/002—Details of machines, plants or systems, using electric or magnetic effects by using magneto-caloric effects
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02B—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO BUILDINGS, e.g. HOUSING, HOUSE APPLIANCES OR RELATED END-USER APPLICATIONS
    • Y02B30/00—Energy efficient heating, ventilation or air conditioning [HVAC]

Definitions

  • the present application relates to a building unit for a heat exchanger block for a magnetocaloric heat exchanger, to magnetocaloric heat exchangers comprising a heat exchanger block comprising two or more of said building units, as well as to processes for manufacturing said building units and said magnetocaloric heat exchangers.
  • Magnetocaloric materials and magnetocaloric heat exchangers are known in the art, see e.g. WO 2011/018348 A2, US 8,763,407 B2 and FR 3 004 795.
  • the present invention relates to a building unit for a magnetocaloric heat exchanger,
  • said building unit comprising a shaped body made up of a one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials, said shaped body comprising
  • a base plate said base plate having a first surface and a second surface opposite to each other
  • said base plate has a base plate thickness B
  • said ridges have a height H
  • At least one of said grooves has a width C of 200 pm or less, preferably of 100 pm or less, more preferably of 50 pm or less, measured at half of height H
  • At least one of said ridges has a width W of 200 pm or less, preferably of 100 pm or less, more preferably of 50 pm or less, measured at half of height H
  • said building unit comprises a shaped body made up of a one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials.
  • Said binding agent binds said particles of said one or more magnetocaloric materials within said shaped body.
  • said binding agent forms a matrix wherein said particles of one or more magnetocaloric material are embedded.
  • said binding agent is in a cured state.
  • Said shaped body comprises a base plate, said base plate having a first surface and a second surface opposite to each other.
  • a fluid flow structure allowing for the flow of a heat transfer medium (herein also referred to as a heat transfer fluid) along predetermined flow paths.
  • Said fluid flow structure comprises two or more parallel ridges protruding from said base plate and one or more grooves each extending between two of said ridges. Said grooves allow for flow of a heat transfer fluid. Each groove has two adjacent ridges confining said groove.
  • the ridges protruding from said base plate and the grooves extending between said ridges cover a large part of the first surface of said shaped body, so that a large number of grooves with adjacent ridges extend over said first surface of said shaped body.
  • the second surface of said base plate of said shaped body is at substantially even level, i.e. has no protrusions and no recesses.
  • each groove and grooves have a rectangular cross section, i.e., each groove has a bottom area extending substantially parallel to the second surface of said base plate and two walls extending substantially perpendicular to the second surface of said base plate, and each ridge has a top area extending substantially parallel to the second surface of said base plate.
  • said second surface of said base plate is the surface of the base plate which faces away from the fluid flow structure.
  • the cross section of each groove has a dip and two walls, and the cross section of each ridge has a peak.
  • Said base plate has a base plate thickness B which corresponds to the perpendicular distance between the second surface of said base plate (i.e. the surface of the base plate which faces away from the fluid flow structure) and the height level of the bottom resp. dip of a groove.
  • said base plate thickness B is in the range of from 10 pm to 200 pm, preferably 10 pm to 100 pm, more preferably 10 pm to 50 pm.
  • Said ridges each have a height H which corresponds to the perpendicular distance (perpendicular with respect to the second surface of the base plate) between the height level of the bottom resp. dip of a groove adjacent to said ridge and the height level of the top area resp. peak of said ridge.
  • Said height H is 200 pm or less, preferably in the range of from 10 pm to 100 pm, preferably of from 20 pm to 50 pm.
  • base plate thickness B and height H of the ridges is substantially constant throughout the whole shaped body.
  • said base plate thickness B is substantially constant throughout the whole shaped body, and all ridges have the same height H. Accordingly, said bottoms resp. dips of all grooves are substantially at the same height level respective to the second surface of the base plate.
  • At least one of said grooves has a width C of 200 pm or less, preferably of 100 pm or less, more preferably of 50 pm or less, measured at half of height H
  • At least one of said ridges has a width W of 200 pm or less, preferably of 100 pm or less, more preferably of 50 pm or less, measured at half of height H
  • all grooves have a width C of 200 pm or less, preferably of 100 pm or less, more preferably of 50 pm or less, measured at half of height H, wherein preferably all grooves have the same width C
  • - all ridges have a width W of 200 pm or less, preferably of 100 pm or less, more preferably of 50 pm or less, measured at half of height H, wherein preferably all ridges have the same width W
  • the fluid flow structure as described herein consists of very fine structures, which due to the plurality of tiny channels and narrow but relatively high (in relation to their width W) ridges provides for a large interface area between the magnetocaloric material and the heat transfer fluid as well as for short heat conducting pathways and for a low pressure drop of the fluid flow.
  • FIGS 1a and 1 b show side views of examples of a shaped body 1 as described above.
  • Said shaped body 1 comprises a base plate 2, said base plate 2 having a first surface 2a and a second surface 2b opposite to each other.
  • a fluid flow structure comprising a plurality of ridges 3 protruding from said base plate 2 and a plurality of grooves 4 each extending between two of said ridges 3.
  • Said second surface 2b of said base plate 2 of said shaped body 1 is at substantially even level, i.e. has no protrusions and no recesses.
  • each groove 4 has a bottom area extending substantially parallel to the second surface 2b of said base plate 2 and two walls extending substantially perpendicular to the second surface 2b of said base plate 2, and each ridge 3 has a top area extending substantially parallel to the second surface 2b of said base plate 2.
  • the bottoms of all grooves 4 are substantially at the same height level respective to the second surface 2b of base plate 2.
  • the top areas of all ridges 3 are substantially at the same height level respective to the second surface 2b of base plate 2.
  • Said base plate 2 has a base plate thickness B which corresponds to the perpendicular distance between the second surface 2b of said base plate 2 (i.e.
  • Said ridges 3 each have a height H which corresponds to the perpendicular distance between the height level of the bottoms of said grooves 4 and the height level of the top areas of said ridges 3.
  • the base plate thickness B is substantially constant over the whole shaped body 1 , and all ridges 3 have the same height H.
  • the grooves 4 have a width C measured at half of height H, and the ridges 3 have a width W measured at half of height H, wherein 0.5 ⁇ H/B ⁇ 2 0.5 ⁇ H/C ⁇ 2 0.5 ⁇ H/W ⁇ 2.
  • each groove 4 has a dip (deepest point of the cross section of said groove) and two walls partly extending in a direction substantially perpendicular to the second surface 2b of said base plate 2, and the cross section of each ridge 3 has a peak (highest point of the cross section of said groove).
  • the dips of all grooves 4 are substantially at the same height level respective to the second surface 2b of base plate 2.
  • the peaks of all ridges 3 are substantially at the same height level respective to the second surface 2b of base plate 2.
  • Said base plate 2 has a base plate thickness B which corresponds to the perpendicular distance between the second surface 2b of said base plate 2 (i.e. the surface of the base plate 2 which faces away from the fluid flow structure) and the height level of the dips of the grooves 4.
  • Said ridges 3 each have a height H which corresponds to the perpendicular distance between the height level of the dips of said grooves 4 and the height level of the peaks of said ridges 3.
  • the base plate thickness B is substantially constant over the whole shaped body 1 , and all ridges 3 have the same height H.
  • the grooves 4 have a width C measured at half of height H, and the ridges 3 have a width W measured at half of height H wherein, 0.5 ⁇ H/B ⁇ 2, 0.5 ⁇ H/C ⁇ 2, 0.5 ⁇ H/W ⁇ 2.
  • said ridges extend continuously from one edge to another edge (typically the opposite edge) of the first surface of said base plate. This type of building unit is advantageous due to its uncomplicated structure which reduces the efforts for manufacturing such building unit.
  • Figure 2 shows a plane view (view from above) of an example of a shaped body 1 having a fluid flow structure as described above.
  • Said fluid flow structure comprises a plurality of parallel ridges 3 extending continuously from one edge to the opposite edge of the first surface 2a of base plate 2, thereby defining a plurality of grooves 4 extending continuous- ly from one edge to the opposite edge of the first surface 2a of a base plate 2.
  • Said grooves 4 act as channels for the flow of a heat transfer fluid.
  • said fluid flow structure comprises
  • the ridges do not extend continuously from one edge to anoth- er edge of said base plate, because the first surface of the base plate is partially covered by one or more regions without protruding ridges. Said regions without protruding ridges are even and are at the same height level relative to the second surface of the base plate like the bottoms resp. dips of said grooves which open out into said region without protruding ridges. In the direction of fluid flow, regions having parallel ridges protruding from said base plate and grooves extending between said ridges alternate with regions without protruding ridges.
  • such region without protruding ridges has a dimension extending parallel to the width C of said grooves which is significantly larger than the width C of said grooves.
  • said region without protruding ridges is of rectangular shape. Said regions without protruding ridges act as fluid redistribution regions, i.e. they allow intermixing of the fluid flow streams emerging from the plurality of grooves which open out into said region without protruding ridges. Due to the fluid redistribution achieved by means of said fluid redistribution region, any risk of channeling and inhomogeneous distribution of the heat transfer fluid is significantly reduced.
  • said fluid flow structure comprises at least
  • first region having a plurality of parallel ridges protruding from said base plate and grooves extending between said ridges
  • second region having a plurality of parallel ridges protruding from said base plate and grooves extending between said ridges
  • said region without protruding ridges which extends between said first region having protruding ridges and said second region having protruding ridges is of rectangular shape, and the long sides of said rectangular region without protruding ridges extend perpendicularly to the ridges in said first region having protruding ridges and perpendicu- larly to the ridges in said second region having protruding ridges.
  • the width Z of said rectangular region (corresponding to the length of the short sides of said rectangle region) without protruding ridges defines the distance between said first region having protruding ridges and said second region having protruding ridges.
  • said distance is small compared to the length L of the grooves in said first region having protruding ridges and to the length of the grooves in said second region having protruding ridges, more specifically preferably 25 % or less of the length of the grooves in said first region having protruding ridges and in said second region having protruding ridges.
  • Figure 3 shows a plan view (view from above) of an example of shaped body 1 having a fluid flow structure as described above.
  • Said fluid flow structure comprises three regions having parallel ridges 3a, 3b, 3c protruding from said base plate 2 and grooves 4a, 4b, 4c extending between said ridges 3a, 3b, 3c, and two fluid redistribution regions 5a, 5b which are regions without protruding ridges.
  • regions having parallel ridges 3a, 3b, 3c protruding from base plate 2 and grooves 4a, 4b, 4c extending between said ridges 3a, 3b, 3c alternate with fluid redistribution regions 5a, 5b.
  • Said fluid redistribution regions 5a, 5b are at the same height level (relative to the second surface of the base plate) like the bottoms resp. dips of said grooves 4a, 4b, 4c which open out into said fluid redistribution regions 5a, 5b.
  • Fluid redistribution region 5a extends between a first region having protruding ridges 3a and a second region having protruding ridges 3b.
  • Fluid redistribution region 5b extends between a first region having protruding ridges 3b and a second region having protruding ridges 3c.
  • Each fluid redistribution regions 5a, 5b is of rectangular shape.
  • the long sides of said rectangular fluid redistribution regions 5a, 5b extend perpendicularly to the ridges 3a, 3b, 3c.
  • the grooves 4a extending between protruding ridges 3a open out into one long side of rectangular fluid redistribution region 5a
  • the grooves 4b extending between protruding ridges 3b open out into the opposite long side of rectangular fluid redistribution region 5a.
  • the grooves 4b extending between protruding ridges 3b open out into one long side of rectangular fluid redistribution region 5b
  • the grooves 4c extending between protruding ridges 3c open out into the opposite long side of rectangular fluid redistribution region 5b.
  • the width Z of said rectangular fluid redistribution region 5a defines the distance between said region having protruding ridges 3a and said region having protruding ridges 3b.
  • the width Z of said rectangular fluid redistribution region 5b defines the distance between said region having protruding ridges 3b and said region having protruding ridges 3c. In both cases, Z is small compared to the length L of the grooves 4a, 4b, 4c, more specifically less than 25 % of the length of the grooves 4a, 4b, 4c.
  • said shaped body is made up of one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials.
  • each mixture comprises a binding agent and particles of one magnetocaloric material.
  • each mixture consists of a binding agent and particles of one magnetocaloric material.
  • said magnetocaloric materials are preferably selected from the group consisting of
  • A represents one or more elements selected from the group consisting of Mn, Co,
  • Z represents one or more elements selected from the group consisting of B, C, Se,
  • x is a number from 0.7 to 0.95
  • y is a number from 0 to 3;
  • x is a number from 0.7 to 0.95
  • y is a number from 0.05 to 1 - x
  • z is a number from 0.005 to 0.5
  • x is a number from 1.7 to 1.95
  • Z is selected from the group consisting of Cr, Cu, Zn, Co, V, As, Ge, x is from 0.01 to 0.5,
  • Z is selected from the group consisting of Cr, Cu, Zn, Co, V, Ge,
  • x is from 0.01 to 0.5.
  • said magnetocaloric materials are selected from the group consisting of compounds of the general formula (I) as defined above. Most preferred are compounds of the general formula (I)
  • A represents Mn, and optionally one or more elements selected from the group consisting of Co, Cr and Ni,
  • Z represents Si and optionally one or more elements selected from the group con- sisting of B, C and N
  • a compound of general formula (I) typically comprises a main phase having an Fe 2 P- structure. Usually said main phase occupies 90 % or more of the volume of said compound of general formula (I).
  • Compounds of general formula (I) and methods for preparation thereof are known in the art. Magnetocaloric materials which contain manganese, iron, silicon and phosphorus, and methods for their preparation are disclosed in WO 2011/083446A1 and US 2011/0220838 A1.
  • Preferred magnetocaloric materials of a composition according to formula (I) which contain manganese, iron, silicon and phosphorus, have a composition according to formula (la)
  • Magnetocaloric materials which contain manganese, iron, silicon, phosphorus, and boron, and methods for their preparation are disclosed in WO 2015/018610, WO 201/018705 and WO 2015/01867.
  • Magnetocaloric materials which contain manganese, iron, silicon, phosphorus, nitrogen and optionally boron and methods for their preparation are disclosed in WO2017/072334.
  • Preferred magnetocaloric materials of a composition according to formula (I), which contain manganese, iron, silicon, phosphorus and nitrogen have a composition according to formula (Id)
  • Preferred magnetocaloric materials of a composition according to formula (I), which contain manganese, iron, silicon, phosphorus, nitrogen and boron have a composition according to formula (le)
  • Magnetocaloric materials which contain manganese, iron, silicon, phosphorus, carbon, and optionally one or both of boron and nitrogen, and methods for their preparation are disclosed in a patent application having the application number PCT/EP2017/063901.
  • Preferred magnetocaloric materials of a composition according to formula (I), which contain manganese, iron, silicon, phosphorus and carbon, have a composition according to formula (If)
  • Preferred magnetocaloric materials of a composition according to formula (I), which contain manganese, iron, silicon, phosphorus, carbon and boron, have a composition according to formula (Ig)
  • Preferred magnetocaloric materials of a composition according to formula (I), which contain manganese, iron, silicon, phosphorus, carbon and nitrogen, have a composition according to formula (Ih)
  • Preferred magnetocaloric materials of a composition according to formula (I), which contain manganese, iron, silicon, phosphorus, carbon, boron and nitrogen, have a composition according to formula (li)
  • said magnetocaloric materials comprise, more preferably consist of particles having a size distribution characterized by
  • the D90 value is 10 pm or less
  • the D50 value is 6 pm or less
  • the D10 value is 2 pm or less.
  • Said particles are spherical or non-spherical or a mixture of both.
  • d is determined by the smallest cross-sectional dimension of said particle.
  • non-spherical particles obtained by crushing larger objects of the corresponding magne- tocaloric material are used, because producing spherical particles is a rather elaborate process, which may suffer from a low yield.
  • the optimal particle size is determined by the dimensions of the fluid flow structure to be obtained, i.e.
  • Said binding agent is preferably selected from the group consisting of polyester polyurethanes having a glass transition temperature in the range of from -45 °C to -5 °C.
  • the glass transition temperature is determined by differential scanning calorimetry (DSC). Determination of glass transition temperatures by means of DSC is known in the art.
  • Polyester polyurethanes are known in the art.
  • the diol com- ponent is selected from the group of polyesters.
  • said binding agent is in the cured state.
  • the total weight fraction of the particles of said magnetocaloric materials is in the range of from 90 wt.-% to 98 wt.-%, more preferably from 92 wt.-% to 97 wt.-%, based on the total weight of said particles of magnetocaloric materials and said binding agent.
  • a high weight fraction of the particles of magnetocaloric materials is desir- able in order to achieve a high magnetocaloric density for the sake of efficient use of the magnetic field volume.
  • a certain amount of binding agent is indispens- ible in order to allow for embedding of the particles of said magnetocaloric material into a matrix formed from said binding agent, thereby holding together said particles and main- taining the desired shape of the shaped body.
  • the whole shaped body is made up of one single mixture comprising a binding agent and particles of one or more magnetocaloric materials, preferably particles of one magnetocaloric material.
  • This type of building unit is advantageous due to its uncomplicated composition which reduces the efforts for manufacturing such building unit.
  • said shaped body consists of three or more portions each comprising particles of a magnetocaloric material having a different Curie temperature, wherein said portions are arranged alongside each other by ascending or descending Curie temperature Tc of the magnetocaloric materials in the direction of the ridges and grooves of the fluid flow structure, wherein in each case the difference between the Curie temperatures of the magnetocaloric materials of two adjacent portions is in the range of from 0.5 K to 4 K.
  • said shaped body consists of three or more portions each made up of a mixture comprising a binding agent and particles of a magneto- caloric material, wherein said magnetocaloric materials of said different mixtures each have a different Curie temperature.
  • said three or more portions are arranged alongside each other by ascending or descending Curie temperature Tc of the magnetocaloric materials in the direction of the ridges and grooves of the fluid flow structure (i.e. in the direction of the flow of the heat transfer fluid). Accordingly, said three or more portions are arranged alongside each other by ascending or descending Curie temperature Tc of the magnetocaloric materials in the flow direction of the heat transfer fluid.
  • the difference between the Curie temperatures of the magnetocaloric materials of two adjacent portions is in the range of from 0.5 K to 4 K.
  • 3 to 40 portions typically each in are in the form of a rectangular stripe having a width of 0.1 to 10 mm, are arranged alongside each other by ascending or descending Curie temperature Tc of the magnetocaloric materials in the direction of the ridges and grooves of the fluid flow structure (i.e. in the direction of the flow of the heat transfer fluid). Accordingly, the length direction of said stripes extends perpendicular to the grooves and ridges of the fluid flow structure, and the heat transfer fluid flows perpendicular to the length direction of stripes.
  • the heat transfer fluid passes portions each made up of a different mixture comprising a binding agent and particles of a magnetocaloric material, wherein said magnetocaloric materials of said different mixtures each have a different Curie temperature.
  • each groove extends over a plurality of such stripes. This is especially the case for building units having shaped bodies with ridges and grooves extending continuously from one edge to another edge of the base plate.
  • each of said regions may be arranged on an individual portion comprising a magnetocaloric material having a different Curie temperature wherein in each case the difference between the Curie temperatures of the magnetocaloric materials of two adjacent portions is in the range of from 0.5 K to 4 K.
  • Figure 4 shows a side view and a plan view (view from above) of an example of a shaped body 1 consisting of three rectangular portions 1a, 1 b, 1c, each comprising particles of a magnetocaloric material having a different Curie temperature.
  • the magnetocaloric material in portion 1a has Curie temperature Tc1
  • the magnetocaloric material in portion 1 b has Curie temperature Tc2
  • the magnetocaloric material in portion 1 b has Curie temperature Tc3.
  • Said three portions 1a, 1 b, 1c are arranged alongside each other by ascending or descending Curie temperature Tc of the magnetocaloric materials in the direction of the ridges 3 and grooves 4 of the fluid flow structure (In the side view said ridges and groves are not visible, because they extend parallel to the plane of the paper). Accordingly, said three portions 1a, 1 b, 1 c are arranged alongside each other by ascending or descending Curie temperature Tc of the magnetocaloric materials in the flow direction of the heat transfer fluid. In each case the difference between the Curie temperatures of the magnetocaloric materials of two adjacent portions is in the range of from 0.5 K to 4 K.
  • Tc1 differs from Tc2 by 0.5 K to 4 K
  • Tc2 differs from Tc3 by 0.5 K to 4 K
  • a building unit having a shaped body consisting of three or more portions each comprising particles of a magnetocaloric material having a different Curie temperature, wherein said portions are arranged alongside each other by ascending or descending Curie temperature Tc of the magnetocaloric materials in the flow direction of the heat transfer fluid as described above is advantageous because by combining magnetocaloric materials having different Curie temperatures the temperature span wherein a magnetocaloric device may provide efficient cooling resp. heating is increased, compared to a magnetocaloric device comprising a single magnetocaloric material.
  • a magnetocaloric heat exchanger preferably comprises three or more different magnetocaloric materials arranged in succession by ascending or descending Curie temperature along the flow path of the heat transfer fluid, i.e.
  • the magnetocaloric material having the highest Curie temperature is arranged at one end of the flow path of the heat transfer fluid, the magnetocaloric material having the second highest Curie temperature follows and so on, and the magnetocaloric material having the lowest Curie temperature is placed at the opposite end of the flow path of the heat transfer fluid.
  • the end of the flow path of the heat transfer fluid where the magnetocaloric material having the highest Curie temperature is located corresponds to the hot side of the magnetocaloric heat exchanger
  • the end of the flow path of the heat transfer fluid where the magnetocaloric material having the lowest Curie temperature is located corresponds to the cold side of the magnetocaloric heat exchanger.
  • each magnetocaloric material (with the exception of the first one) to a temperature near its Curie temperature is effected by the preceding magnetocaloric material, and each magnetocaloric material (with the exception of the last one) effects cooling resp. heating of the succeeding magnetocaloric material to a temperature near its Curie temperature.
  • the first magnetocaloric material effects cooling down resp. heating up the second magnetocaloric material to a temperature near the Curie temperature of the second magnetocaloric material, and so on with any further magnetocaloric material contained in the cascade.
  • the cooling effect achieved can be greatly increased in comparison with a magnetocaloric heat exchanger comprising a single magnetocaloric material.
  • the number of different magnetocaloric materials and their Curie temperatures are se- lected depending on the temperature span to be covered in the desired application.
  • the difference in the Curie temperatures between the magnetocaloric material with the highest Curie temperature and the magnetocaloric material with the lowest Curie temperature corresponds to said temperature span.
  • the Curie temperature of a magnetocaloric material depends on the chemical composi- tion of the magnetocaloric material.
  • the above-mentioned three or more magnetocaloric materials having a different Curie temperature may be magnetocaloric materials having different chemical composition.
  • magnetocaloric materials especially for those of above-defined general formula (I), it is well-known that slight variation of the stoichiometry (i.e. of the proportions between the different elements present in said material) has a significant influence on the Curie temperature.
  • magnetocaloric materials having different Curie temperatures at identical stoichiometry are obtainable by varying the temperature of the heat treatment applied in the preparation of such materials, as described in non-prepublished patent application of application number PCT/EP2017/071885.
  • said building unit consists of a shaped body as defined above, preferably a shaped body having one or more of the above-defined preferred features. This type of building unit is advantageous due to the absence of parts made up of materials which do not contribute to the magnetocaloric effect.
  • said building unit comprises a shaped body as defined above, preferably a shaped body having one or more of the above-defined preferred features, and a substrate which does not comprise any magnetocaloric material, said substrate having a first surface and a second surface opposite to each other, wherein said first surface of said substrate is attached to the second surface of the base plate of said shaped body.
  • said building unit further comprises a second shaped body as defined above, preferably a shaped body having one or more of the above-defined preferred features, wherein said second surface of said substrate is attached to the second surface of the base plate of said second shaped body.
  • said preferred type of building unit comprises a shaped body as defined above, preferably a shaped body having one or more of the above- defined preferred features, and a substrate which does not comprise any magnetocaloric material, wherein said substrate is attached to the second surface of the base plate of said shaped body.
  • This type of building unit is advantageous, because the substrate imparts mechanical stability to the shaped body to which it is attached, and facilitates handling of the building unit.
  • said second surface of said base plate of said shaped body is at substantially even level, i.e. has no protrusions and no recesses.
  • the substrate usually origins from the method of manufacturing a building unit according to the present invention, see third aspect of the present invention as described below.
  • a building unit of the above-defined type consists of a shaped body as defined above, preferably a shaped body having one or more of the above-defined preferred features, and a substrate which does not comprise any magnetocaloric material, wherein said substrate is attached to the second surface of the base plate of said shaped body.
  • FIG. 5 shows a side view of an example of a building unit of the above-defined type.
  • Said building unit 100 consists of a shaped body 1 as defined above, preferably a shaped body having one or more of the above-defined preferred features, and a substrate 11 which does not comprise any magnetocaloric material.
  • Said substrate 11 is attached to the second surface 2b of the base plate 2 of said shaped body 1.
  • a building unit of the above-defined type comprises a first shaped body and a second shaped body as defined above, and a substrate which does not comprise any magnetocaloric material, said substrate having a first surface and a second surface opposite to each other, wherein said first surface of said substrate is attached to the second surface of the base plate of said first shaped body and said second surface of said substrate is attached to the second surface of the base plate of said second shaped body.
  • said first shaped body and said second shaped body preferably have one or more of the above-defined preferred features.
  • the second surface of the base plate of said first shaped body is at substantially even level, i.e.
  • This type of building unit is advantageous, because one substrate imparts mechanical stability to two shaped bodies attached to said substrate, thereby reducing the volume fraction occupied by the substrate (which does not contribute to the magnetocaloric effect) relative to the total volume of substrate and shaped bodies comprising particles of one or more magnetocaloric materials.
  • said first shaped body and said second shaped body are of identical composition, shape, structure and dimensions. More specifically, the fluid flow structures of the first shaped body and the second shaped body are like mirror images with regard to each other.
  • a building unit of the above-defined type consists of a first shaped body and a second shaped body as defined above, and a substrate which does not comprise any magnetocaloric material, said substrate having a first surface and a second surface opposite to each other, wherein said first surface of said substrate is attached to the second surface of the base plate of said first shaped body and said second surface of said substrate is attached to the second surface of the base plate of said second shaped body.
  • Figure 6 shows a side view of an example of a building unit of the above-defined type.
  • Said building unit 200 consists of a first shaped body T as defined above, preferably in the form of a shaped body having one or more of the above-defined preferred features, a second shaped body 1” as defined above, preferably in the form of a shaped body having one or more of the above-defined preferred features, and a substrate 11 which does not comprise any magnetocaloric material.
  • Said substrate 11 has a first surface and a second surface opposite to said first surface . The first surface of said substrate 11 is attached to the second surface 2b’ of the base plate 2’ of said first shaped body T and the second surface of said substrate 11 is attached to the second surface 2b” of the base plate 2” of said second shaped body 1”.
  • the fluid flow structure having protruding ridges 3 and grooves 4’ extending between said protruding ridges of said first shaped body T and the fluid flow structure having protruding ridges 3” and grooves 4” extending between said protruding ridges of said second shaped body 1” are like mirror images with regard to each other.
  • Said substrate is preferably in a form selected from the group consisting of foils, films, webs, panes and plates.
  • said substrate has a thickness in the range of from 0.1 pm to 100 pm, preferably 1 pm to 25 pm more preferably 1 pm to 15 pm, most preferably 1 pm to 10 pm.
  • said substrate comprises one or more materials from the group consisting of organic polymers and metals.
  • Preferred organic polymers are polyethylene terephthalate PET, polyethylene naphthalate PEN, polypropylene PP, polyeth- ylene PE, polyamide, polyimide and Aram id.
  • Preferred metals are aluminum, copper and stainless steel.
  • said substrate is in a form selected from the group consisting of foils, films, webs, panes and plates, has a thickness in the range of from 0.1 pm to 100 pm, preferably 1 pm to 25 pm, more preferably 1 pm to 15 pm, most preferably 1 pm to 10 pm, and comprises one or more materials from the group consisting of organic polymers and metals.
  • the lateral dimensions (dimensions perpendicular to the base plate thickness B) of a building unit according to the present invention are both in the range of from 0.1 mm to 50 mm.
  • the present invention relates to a magnetocaloric heat exchanger comprising a heat exchanger block comprising two or more building units, preferably 50 to 1000 building units, according to the first aspect of the present invention, preferably building units having one or more of the above-defined preferred features, subsequently stacked on top of one another
  • the ridges protruding from the base plate of the shaped body of the first building unit engage the substrate attached to the base plate of the shaped body of the second building unit stacked on top of said first building unit
  • the ridges protruding from the base plate of a shaped body of the first building unit engage the ridges protruding from the base plate of a shaped body of the second building unit stacked on top of said first building unit.
  • each of the stacked building units consists of a shaped body as defined above, preferably a shaped body having one or more of the above-defined preferred features (for examples of such shaped body, see figure 1a and
  • Figure 7a shows an example of a heat exchanger block according to said first preferred type.
  • three building units 10a, 10b, 10c are stacked on top of each other.
  • Each of the stacked building units consists of a shaped body as defined above, preferably a shaped body having one or more of the above-defined preferred features.
  • the ridges protruding from the base plate of the shaped body of the first building unit engage the second surface of the base plate of the shaped body of the second building unit stacked on top of said first building unit.
  • the ridges protruding from the base plate of the shaped body of the lowermost building unit 10a engage the second surface of the base plate of the shaped body of the middle building unit 10b
  • the ridges protruding from the base plate of the shaped body of the middle building unit 10b engage the second surface of the base plate of the shaped body of the uppermost build- ing unit 10c.
  • two or more building units are subsequently stacked on top of one another, so that in each case between two building units stacked one on top of the other the ridges protruding from the base plate of the shaped body of the first building unit engage the substrate attached to the base plate of the shaped body of the second building unit stacked on top of said first building unit.
  • the stacked building units each comprise a substrate.
  • each of the stacked building units consists of a shaped body as defined above, preferably a shaped body having one or more of the above-defined preferred features, and a substrate, preferably a substrate having one or more of the above-defined preferred features, attached to the second surface of the base plate of said shaped body (for an example of such building unit, see figure 5).
  • FIG. 7b shows an example of a heat exchanger block according to said second preferred type.
  • three building units 100a, 100b, 100c are stacked on top of each other.
  • Each of the stacked building units consists of a shaped body as defined above, preferably a shaped body having one or more of the above- defined preferred features and a substrate 11a, 11 b, 11c, preferably a substrate having one or more of the above-defined preferred features, attached to the second surface of the base plate of said shaped body.
  • the ridges protruding from the base plate of the shaped body of the first building unit engage the substrate attached to the base plate of the shaped body of the second building unit stacked on top of said first building unit. More specifically, the ridges protruding from the base plate of the shaped body of the lowermost building unit 100a engage the substrate 1 1 b attached to the base plate of the shaped body of the middle building unit 100b, and the ridges protruding from the base plate of the shaped body of the middle building unit 100b engage the substrate 1 1 c attached to the base plate of the shaped body of the uppermost building unit 100c.
  • two or more building units are subsequently stacked on top of one another, so that the ridges protruding from the base plate of a shaped body of the first building unit engage the ridges protruding from the base plate of a shaped body of the second building unit stacked on top of said first building unit.
  • the stacked building units each comprise a first and a second shaped body as defined above, and a substrate which does not comprise any magnetocaloric material, said substrate having a first and a second surface opposite to each other, wherein said first surface of said sub- strate is attached to the second surface of the base plate of said first shaped body and said second surface of said substrate is attached to the second surface of the base plate of said second shaped body.
  • each building unit has a first (lower) and a second (upper) shaped body, and accordingly a first (lower) and a second (upper) fluid flow structure.
  • each of the stacked building units consists of a first and a second shaped body as defined above, preferably said shaped bodies each having one or more of the above-defined preferred features, and a substrate, preferably a substrate having one or more of the above-defined preferred features, said substrate having a first surface and a second surface opposite to each other, wherein said first surface of said substrate is attached to the second surface of the base plate of said first shaped body and said second surface of said substrate is attached to the second surface of the base plate of said second shaped body (for an example of such building unit, see figure 6).
  • the fluid flow structures of adjacent stacked building units are designed so that fitting of the ridges of the fluid flow structure of one building unit into the grooves of the adjacent fluid flow structure of the adjacent building unit is precluded.
  • This is achieved e.g. by providing said building unit with fluid flow structures wherein the width W of the ridges is larger than the width C of said grooves of the adjacent building unit, thereby precluding that the ridges of the fluid flow structure of one building unit to fit into the grooves of the adjacent fluid flow structure of the adjacent building unit.
  • the ridges of adjacent building units cooperate to define a combined fluid flow structure wherein the adjacent fluid flow structures of two building units stacked on top of the other cooperate with each other.
  • Figures 7c and 7d show examples of a heat exchanger block according to said third preferred type.
  • heat exchanger block 7c resp. 7d in each case three building units 200a, 200b, 200c resp. 200d, 200e, 200f are stacked on top of each other.
  • Each of the stacked building units consists of a first and a second shaped body as defined above, and a substrate 1 1a, 1 1 b, 1 1 c, 1 1 d, 1 1 e, 1 1f which does not comprise any magnetocaloric material, said substrate having a first and a second surface opposite to each other, wherein said first surface of said substrate is attached to the second surface of the base plate of said first shaped body and said second surface of said substrate is attached to the second surface of the base plate of said second shaped body (cf. figure 6).
  • the fluid flow structures of first shaped body and the second shaped body are like mirror images with regard to each other.
  • the ridges protruding from the base plate of a shaped body of the first building unit engage the ridges protruding from the base plate of a shaped body of the second building unit stacked on top of said first building unit. More specifically, the ridges protruding from the base plate of the upper shaped body of the lowermost building unit 200a, 200d engage the ridges protruding from the base plate of the lower shaped body of the middle building unit 200b, 200e, and the ridges protruding from the base plate of the upper shaped body of the middle building unit 200b, 200e engage the ridges protruding from the base plate of the lower shaped body of the uppermost building unit 200c, 200f.
  • figures 7c and 7d differ with regard to the relative positions of the ridges and grooves of adjacent fluid flow structures of building units 200a, 200b, 200c resp. 200d, 200e, 200f.
  • the three building units 200a, 200b, 200c are subsequently stacked on top of one another, so that the positions of the grooves of the fluid flow structure of each building unit are shifted with regard to the positions of the grooves in the adjacent fluid flow structures of the adjacent building units.
  • the grooves of the upper fluid flow structure of the lowermost building unit 200a are shifted with regard to the grooves of the lower fluid flow structure of the middle building unit 200b, so that the grooves of the upper fluid flow structure of the lowermost building unit 200a do not match with the grooves of the lower fluid flow structure of the middle building unit 200b, and the grooves of the upper fluid flow structure of the middle building unit
  • the three building units 200d, 200e, 200f are subsequently stacked on top of one another, so that the grooves of the fluid flow structure of each building unit match with the grooves in the adjacent fluid flow structures of the adjacent building units. More specifically, the grooves of the upper fluid flow structure of the lowermost building unit 200d match with the grooves of the lower fluid flow structure of the middle building unit 200e, and the grooves of the upper fluid flow structure of the middle building unit 200e match with the grooves of the lower fluid flow structure of the uppermost building unit 200f.
  • the height of a heat exchanger block (dimension in the direction in which the building units are stacked on top of each other) is in the range of from 0.1 cm to 4 cm, depending on the thickness of the individual building units and the number of building units. Usually the height of the heat exchanger block is shorter than both of the lateral directions of the building units.
  • Magnetocaloric heat exchangers as such are known in the art, see e.g. WO 201 1/018348 A2, US 8,763,407 B2 and FR 3 004 795.
  • a magnetocaloric heat exchanger according to the present invention may further comprise a casing surrounding said heat exchanger block.
  • the casing can be made of any suitable material. Typically casings are made of plastics such as glass-reinforced polypropylene, carbon-fiber reinforced polyetheretherketone or glass-fiber reinforced epoxy. Metals like steel and aluminum are also possible, but are not preferred.
  • the heat exchanger block is fixed in the casing by means of a two component (2K) epoxy resin.
  • 2K two component
  • a magnetocaloric heat exchanger typically comprises further construction elements. Details thereof are known to the skilled person. Said further construction elements typically comprise means for applying a changing external magnet- ic field to the heat exchanger block and means (typically in the form of tubing and/or piping) for charging and discharging a heat transfer fluid, distributing said heat transfer fluid to the stacked building units in order to allow parallel flow of the heat transfer fluid over the stacked building units, and collecting the heat transfer fluid emerging from the stacked building units over which the hat transfer fluid has flown.
  • the tubing/piping connects the heat exchanger block according to the invention material with the hot side and the cold side of the magnetocaloric heat exchanger.
  • the magnetocaloric heat exchanger according to the present invention is typically installed within a magnetocaloric device, e.g. a magnetocaloric cooling device.
  • This device may be configured to use multiple magnetocaloric heat exchangers which all contribute to the device performance.
  • the present invention relates to a process for manufacturing a building unit as defined above, preferably a building unit having one or more of the above-defined preferred features, for a magnetocaloric heat exchanger, said process comprising the steps
  • a coated substrate having a coating layer made up of one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials disposed on said substrate, said coating layer having a first surface facing away from said substrate and opposite to said first surface a second surface in contact with said substrate
  • each of said mixtures comprises a binding agent and particles of one magnetocaloric material, or consists of one a binding agent and particles of one magnetocaloric material.
  • Preferred magnetocaloric materials are as described above in the context of the first aspect of the present invention.
  • Preferred particle size distribution of the particles of the magnetocaloric materials is as described above in the context of the first aspect of the present invention.
  • Said binding agent is preferably selected from the group consisting of polyester polyurethanes having a glass transition temperature in the range of from -45 °C to -5 °C.
  • polyester polyurethanes exhibit thermoplastic behavior. More specifically, said polyester polyurethanes are ductile and flexible, which allows for tight conformation of the mixture comprising said binding agent selected from the group consisting of the above-defined polyester polyurethanes and particles of one or more magnetocaloric materials to the contours of the embossing roll, so that building units with appropriate contour accuracy can be obtained.
  • the total weight fraction of the particles of said magnetocaloric materials is in the range of from 90 wt.-% to 98 wt.-%, preferably from 92 wt.-% to 97 wt.-%, based on the total weight of said particles of magnetocaloric materials and said binding agent.
  • the mixture comprises further constituents which serve to facilitate processa- biltiy of said mixture, but are removed during processing (mainly during the step of curing) and accordingly are not present in the shaped body finally obtained from said mixture.
  • the mixture comprises a solvent or a mixture of solvents for dissolving the binding agent.
  • Preferred solvents for binding agents selected from the group of polyester polyurethanes as described above are propylene glycol mono methyl ether acetate (PGMEA), ethylacetate, acetone/toluene (volume ratio 2: 1 ) and methylethylketone/ethylacetate (volume ratio 1 :1 ).
  • Preferred solvents for binding agents selected from the group of polyester polyurethanes as described above are propylene glycol mono methyl ether acetate (PGMEA), ethylacetate, acetone/toluene (volume ratio 2: 1 ) and methylethylketone/ethylacetate (volume ratio 1 :1 ).
  • Said substrate is preferably in a form selected from the group consisting of foils, films, webs, panes and plates.
  • said substrate has a thickness in the range of from 0.1 pm to 100 pm, preferably 1 pm to 25 pm, more preferably 1 pm to 15 pm, most pref- erably 1 mih to 10 mih.
  • said substrate comprises one or more materials from the group consisting of organic polymers and metals.
  • Preferred organic polymers are polyethylene terephthalate PET, polyethylene naphthalate PEN, polypropylene PP, polyethylene PE, polyamide, polyimide and Aram id.
  • Preferred metals are aluminum, copper and stainless steel.
  • said substrate is in a form selected from the group consisting of foils, films, webs, panes and plates, has a thickness in the range of from 0.1 pm to 100 pm, preferably 1 pm to 25 pm, more preferably 1 pm to 15 pm, most preferably 1 pm to 10 pm, and comprises one or more materials from the group consisting of organic polymers and metals.
  • said one or more mixtures are applied to said first surface of said substrate, to form a coated substrate having a coating layer made up of one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials disposed the first surface on said substrate.
  • Said coating layer has a first surface facing away from said substrate and opposite to said first surface a second surface in contact with said substrate.
  • FIG. 9 shows an example of a coated substrate 13 as described above.
  • Said coated substrate 13 consists of a coating layer 12 made up of one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials, and a substrate 11.
  • Said substrate 11 has a first surface 1 T and a second surface 11” opposite to each other.
  • Said coating layer 12 is disposed on said first surface 1 T of said substrate 11.
  • Said coating layer has a first surface 12a facing away from said substrate 1 1 and opposite to said first surface 12a a second surface 12b in contact with said substrate 11.
  • said mixtures are applied to said surface of said substrate by means of a coating technique, e.g. slot-die coating.
  • a coating technique e.g. slot-die coating.
  • said coating layer has a thickness in the range of from 30 pm to 200 pm (as measured prior to treating the first surface of said coating layer by means of an embossing roll).
  • said first surface of said coating layer is treated by means of an embossing roll, the surface of said embossing roll exhibiting a structure which is a negative with respect to the fluid flow structure of the building unit to be manufactured.
  • the desired fluid flow structure is imparted to the first surface of the coating layer, thereby transforming the coating layer into a shaped body as defined above.
  • the surface of the embossing roll exhibits a structure which is a negative with respect to the fluid flow structure of the building unit to be manufactured, i.e. a structure which is inverted with regard to the fluid flow structure to be imparted to the surface of the coating layer treated by means of the embossing roll.
  • the structure at the surface of the embossing roll has recessed areas at those positions where the intended fluid flow structure has protruding areas (ridges as defined above) and has protruding areas at those positions where the intended fluid flow structure has recessed areas (grooves as defined above, and optionally fluid redistribution regions i.e. without protruding ridges into which said grooves open out).
  • embossing is achieved by guiding the coated substrate through a pair of cylinder-shaped rolls rotating in opposite direction.
  • this is achieved by a calendaring machine equipped with said pair of rolls.
  • the pair of rolls consists of a first roll acting on the coating layer and a second roll supporting the substrate.
  • Said first roll is the embossing roll.
  • the surface of said embossing roll exhibits a structure which is a negative with respect to the fluid flow structure of the building unit to be manufactured (as explained above).
  • the embossing roll has a core made of copper and disposed on the surface of said core a coating made of hard chromium.
  • the supporting roll has a hard rubber coating.
  • said rubber coating has a thickness in the range of from 0.2 mm to 0.4 mm, preferably 0.25 to 0.25 mm, and a shore D hardness SH 90.
  • embossing is carried out with a line force in the range of from 60 N/mm to 160 N/mm, and the coated substrate moves through the pair of rolls with a speed of 0.1 m/min to 1 m/min, preferably 0.25 m/min to 0.75 m/min, most preferably 0.4 m/min to 0.6 m/min.
  • the em- bossing technique used according to the present invention has the advantage that the entire structure is obtained in a single process cycle, thereby increasing the throughput.
  • manufacturing of structures having a certain thickness by means of 3D printing requires carrying out a large number of printing steps, because the higher the thick- ness of the structure, the larger the number of layers to be printed to build up the desired structure.
  • embossing is carried out as a hot embossing process.
  • said embossing roll is kept at a temperature in the range of from 40 °C to 60 °C, while said sup- porting roll is not heated.
  • Figure 10 shows an example of a setup used in the embossing step of the process according to the present invention.
  • a coated substrate 13 consisting of a substrate 11 and a coating layer 12 made up of one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials disposed on a first surface 1 1’ of a substrate 11 is guided through a pair of cylinder-shaped rolls 15 and 16 rotating in opposite direction.
  • the pair of rolls 15, 16 consists of a first roll 15 acting on the coating layer 12 and a second roll 16 supporting the substrate 1 1.
  • Said first roll 15 is the embossing roll.
  • the surface of said embossing roll exhibits a structure 15a which is a negative with respect to the fluid flow structure of the building unit to be manufactured.
  • the surface of the coating layer 12 exhibits a fluid flow structure comprising ridges 3 and grooves 4 as described above.
  • the binding agent is cured. Whether curing is performed or not, depends on the used binding agent.
  • Use of curable binding agents and curing them after embossing has the advantage of improving the form stability of the fluid flow structure.
  • said binding agent is selected from the group consisting of polyester polyurethanes having a glass transition temperature in the range of from -45 °C to -5 °C, and curing said polyester polyurethane is carried out at a temperature of 200 °C or less, preferably in the range of from 120 °C to 190°C.
  • a building unit according to the present invention is obtained by forming a piece of said coated substrate having lateral dimensions corresponding to said building unit. Usually, this is done by cutting to size said coated substrate, or punching out from the coated substrate a piece of said coated substrate having lateral dimensions corresponding to said building unit.
  • the substrate provided for the above-described process is a substrate already cut to size of the building unit to be manufactured. However, this approach is less preferred because it inhibits performing the steps of coating, embossing and curing in a continuous manner for large areas.
  • a substrate having at least one lateral dimension (usually, a length) significantly larger than a lateral dimension of the building unit to be manufactured, thereby allowing for performing the steps of coating, embossing and curing in a continuous manner for large areas, so that a large number of building units can be obtained when said substrate is processed.
  • said substrate is removed from said second surface of said coating layer.
  • the substrate is preferably peeled off from the coating layer.
  • this is done before forming said piece having lateral dimensions corresponding to said building unit, e.g. before said coated substrate is cut to size.
  • a process according to the present invention, wherein said substrate is removed from said second surface of said coating layer allows for manufacturing a building unit which consists of a shaped body as described above, preferably a shaped body having one or more of the above-defined preferred features. An example of such shaped body is shown in figure 1.
  • said substrate is not removed from said second surface of said coating layer.
  • a process according to the present invention, wherein said substrate is not removed from said second surface of said coating layer allows for manufacturing a building unit which comprises a shaped body as defined above, preferably a shaped body having one or more of the above-defined preferred features, and a substrate which does not comprise any magnetocaloric material, said substrate having a first and a second surface opposite to each other, wherein said first surface of said substrate is attached to the second surface of the base plate of said shaped body.
  • An example of such a building unit is shown in figure 5.
  • said building unit further comprises a second shaped body as defined above, preferably a shaped body having one or more of the above-defined preferred features, and said second surface of said substrate is attached to the second surface of the base plate of said second shaped body.
  • a process according to the invention wherein said substrate is not removed from said second surface of said coating layer, said process comprising the steps of
  • a coated substrate having a first coating layer made up of one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials disposed on said first surface of said substrate, and a second coating layer made up of one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials disposed on said second surface of said substrate, each of said coating layers having a first surface facing away from said substrate and opposite to said first surface a second surface in contact with said substrate
  • This preferred process according to the present invention allows for manufacturing a building unit which comprises a first and a second shaped body as defined above, and a substrate which does not comprise any magnetocaloric material, said substrate having a first and a second surface opposite to each other, wherein said first surface of said substrate is attached to the second surface of the base plate of said first shaped body and said second surface of said substrate is attached to the second surface of the base plate of said second shaped body.
  • An example of such a building unit is shown in figure 6.
  • one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials are provided, and a substrate which does not comprise any magnetocaloric material, said substrate having a first and a second surface opposite to each other, is provided.
  • P re- ferred mixtures and substrates are as described above.
  • said one or more mixtures are applied to said first surface and to said second surface of said substrate, to form a coated substrate having a first coating layer made up of one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials dis- posed on said first surface of said substrate, and a second coating layer made up of one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials disposed on said second surface of said substrate.
  • Each of said coating layers has a first surface facing away from said substrate and opposite to said first sur- face a second surface in contact with said substrate.
  • Figure 11 shows an example of a coated substrate 14 as described above.
  • Said coated substrate 14 consists of a first coating layer 12’ made up of one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials, a second coating layer 12” made up of one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials, and a substrate 11.
  • Said substrate 11 has a first surface 11’ and a second surface 11” opposite to each other.
  • Said first coating layer 12’ is disposed on said first surface 1 1’ of said substrate 11.
  • Said second coating layer 12” is disposed on said second surface 1 1” of said substrate 1 1.
  • Said first coating layer 12’ has a first surface 12a’ facing away from said substrate 11 and opposite to said first surface 12a’, a second surface 12b’ in contact with said first surface 11’ of said substrate 1 1.
  • Said second coating layer 12 has a first surface 12a” facing away from said substrate 1 1 and opposite to said first surface 12a”, a second surface 12b” in contact with said second surface 11” of said substrate 11.
  • said mixtures are applied to said first and said second surface of said sub- strate by means of a coating technique, e.g. slot-die coating.
  • a coating technique e.g. slot-die coating.
  • said first and second coating layer has a thickness in the range of from 30 pm to 200 pm (as measured prior to treating the first surface of said first coating layer and the first surface of said second coating layer, resp., by means of an embossing roll).
  • said first coating layer and said second coating layer have substantially the same thickness.
  • the first surface of said first coating layer and the first surface of said second coating layer are each treated by means of an embossing roll, the surface of said embossing roll in each case exhibiting a structure which is a negative with respect to the fluid flow structure of the building unit to be manufactured.
  • the desired fluid flow structure is imparted to the first surface of the first coating layer, thereby transforming the first coating layer into a first shaped body as defined above
  • the desired fluid flow structure is imparted to the first surface of the second coating layer, thereby transforming the second coating layer into a second shaped body as defined above.
  • embossing of the coated substrate is done by means of a pair of structured embossing rollers, one acting on the first surface of said first coating layer, the other one acting on the first surface of said second coating layer.
  • the fluid flow structures which are imparted to said first coating layer and said second coating layer are like mirror images with regard to each other.
  • Figure 12 shows an example of a setup used in the embossing step of the above-defined preferred process according to the present invention.
  • a coated substrate 14 (cf.
  • figure 1 1 consisting of a substrate 1 1 , first coating layer 12’ made up of one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials disposed on a first surface 1 1’ of said substrate and a second coating layer 12” made up of one or more mixtures each comprising a binding agent and particles of one or more magnetocaloric materials disposed on a second surface 1 1” of said substrate a is guided through a pair of cylinder-shaped rolls 15’ and 15” rotating in opposite direction.
  • the pair of rolls 15’, 15” consists of a first embossing roll 15’ acting on the first coating layer 12’ and a second embossing roll 15” acting the second coating layer 12”.
  • the surfaces of said embossing rolls 15’, 15” exhibit structures 15a’, 15a” which are a negative with respect to the fluid flow structure of the building unit to be manufactured.
  • the surface of the first coating layer 12’ exhibits a fluid flow structure comprising ridges 3’ and grooves 4’ as described above
  • the surface of the second coating layer 12 exhibits a fluid flow structure comprising ridges 3” and grooves 4” as described above.
  • the fluid flow structure on the first coating layer 12’ and the fluid flow structure on the second coating layer 12” are like mirror images with regard to each other.
  • the binding agent is cured. Whether curing is performed or not, depends on the used binding agent.
  • the binding agent is selected from the group consisting of polyester polyurethanes having a glass transition temperature in the range of from -45 °C to -5 °C, and curing said polyester polyurethane is carried out at a temperature of 200 °C or less, preferably in the range of from 120 °C to 190°C.
  • a building unit as defined above is obtained as described above by forming a piece of said coated substrate having lateral dimensions corresponding to said building unit. Usually, this is done by cutting to size said coated substrate, or punching out from the coated substrate a piece of said coated substrate having lateral dimensions corresponding to said building unit.
  • only one mixture comprising a binding agent and particles of one or more magnetocaloric materials, preferably particles of one magnetocaloric material, are applied to a surface of said substrate.
  • a building unit comprising a shaped body made up of one mixture comprising a binding agent and particles of one or more magnetocaloric materials, preferably particles of one magnetocaloric material, is obtained.
  • each of said three or more mixtures to a portion of the surface of said substrate by ascending or descending Curie temperature Tc of the magnetocaloric materials to form a coated substrate having a coating layer consisting of three or more portions each comprising particles of a magnetocaloric material having a dif- ferent Curie temperature disposed on said substrate, wherein said three or more portions are arranged alongside each other by ascending or descending Curie temperature Tc of the magnetocaloric materials, wherein in each case the difference between the Curie temperatures of the magnetocaloric materials of two adjacent portions is in the range of from 0.5 to 4 K, said coating layer having a first sur- face facing away from said substrate and opposite to said first surface a second surface in contact with said substrate,
  • This preferred process according to the present invention allows for manufacturing a building unit according to the present invention comprising a shaped body, wherein said shaped body consists of three or more portions each comprising particles of a magnetocaloric material having a different Curie temperature, wherein said portions are arranged alongside each other by ascending or descending Curie temperature Tc of the magnetocaloric materials in the direction of the ridges and grooves of the fluid flow structure, wherein in each case the difference between the Curie temperatures of the magnetocaloric materials of two adjacent portions is in the range of from 0.5 K to 4 K.
  • Tc Curie temperature
  • three or more mixtures each comprising a binding agent and particles of one magnetocaloric material are provid- ed, wherein in each mixture the magnetocaloric material has a different Curie temperature, and a substrate which does not comprise any magnetocaloric material, said substrate having a first and a second surface opposite to each other, is provided.
  • Preferred mixtures and substrates are as described above.
  • each of said three or more mixtures is applied to an individual portion of said surface of said substrate by ascending or descending Curie temperature Tc of the magnetocaloric materials.
  • Tc Curie temperature
  • the first mixture comprising a magnetocaloric material having the highest resp. lowest Curie temperature is applied to a first portion of the surface of said substrate
  • the second mixture comprising a magnetocaloric material having the next higher resp. lower Curie tem- perature with respect to the magnetocaloric material in the first mixture is applied to a second portion alongside said first portion of the surface of said substrate, the third mixture comprising a magnetocaloric material having the next higher resp.
  • a coated substrate having a coating layer consisting of three or more portions each comprising particles of a magnetocaloric material having a different Curie temperature disposed on said substrate.
  • said three or more portions are arranged alongside each other by ascending or descending Curie temperature Tc of the magnetocaloric materials.
  • the magnetocaloric materials are selected so that in each case the difference between the Curie temperatures of the magnetocaloric materials of two adjacent portions is in the range of from 0.5 K to 4 K.
  • Said coating layer has a first surface facing away from said substrate and opposite to said first surface a second surface in contact with said substrate.
  • said mixture is applied to said surface of said substrate by means of a coating technique, e.g. slot-die coating.
  • said layer has a thickness in the range of from 30 pm to 200 pm (as measured prior to treating the first surface of said coating layer by means of an embossing roll.)
  • the first surface of said coating layer is treated by means of an embossing roll, the surface of said embossing roll exhibiting a structure which is a negative with respect to the fluid flow structure of the building unit to be manufactured.
  • Treating the first surface of said coating layer by means of an embossing roll is carried out so that the ridges and grooves of the fluid flow struc- ture extend perpendicular to said three or more portions each comprising particles of a magnetocaloric material having a different Curie temperature.
  • the desired fluid flow structure is imparted to the first surface of the coating layer thereby transforming the coating layer into a shaped body as defined above.
  • An example of such shaped body is shown in figure 4.
  • said embossing roll is kept at a temperature in the range of from 40 °C to 60 °C.
  • the binding agent in the coating layer is cured. Whether curing is per- formed or not depends on the used binding agent.
  • Use of curable binding agents and curing them after embossing is performed has the advantage of improving the form stability of the fluid flow structure.
  • said binding agent is selected from the group consisting of polyester polyurethanes having a glass transition temperature in the range of from -45 °C to -5 °C, and curing said polyester polyurethane is carried out at a temperature of 200 °C or less, preferably in the range of from 120 °C to 190°C.
  • a building unit as defined above is obtained as described above by forming a piece of said coated substrate having lateral dimensions corresponding to said building unit. Usually, this is done by cutting to size said coated substrate, or punching out from the coated substrate a piece of said coated substrate having lateral dimensions corresponding to said building unit.
  • the present invention relates to a process for manufacturing a magnetocaloric heat exchanger, comprising the steps of
  • the ridges protruding from the base plate of the shaped body of the first building unit engage the substrate attached to the base plate of the shaped body of the second building unit stacked on top of said first building unit or
  • the ridges protruding from the base plate of a shaped body of the first building unit engage the ridges protruding from the base plate of a shaped body of the second building unit stacked on top of said first building unit.
  • a heat exchanger block is formed by subsequently stacking said building units on top of one another.
  • said two or more, preferably 50 to 1000 building units are those which have one or more of the above-defined preferred features.
  • the two or more building units are subsequently stacked on top of one another, so that in each case between two building units stacked one on top of the other the ridges protruding from the base plate of the shaped body of the first building unit engage the second surface of the base plate of the shaped body of the second building unit stacked on top of said first building unit.
  • the stacked building units do not comprise a substrate.
  • each of the stacked building units consists of a shaped body as defined in above, preferably a shaped body having one or more of the above-defined preferred features.
  • An example of a stack obtainable in this manner is shown in figure 7a.
  • the two or more building units are subsequently stacked on top of one another, so that in each case between two building units stacked one on top of the other the ridges protruding from the base plate of the shaped body of the first building unit engage the substrate attached to the base plate of the shaped body of the second building unit stacked on top of said first building unit.
  • the stacked building units each comprise a substrate.
  • each of the stacked building units consists of a shaped body as defined in above, preferably a shaped body having one or more of the above-defined preferred features, and a substrate, preferably a substrate having one or more of the above-defined preferred features, attached to the second surface of the base plate of said shaped body.
  • a stack obtainable in this manner is shown in figure 7b.
  • the two or more building units are subsequently stacked on top of one another, so that the ridges protruding from the base plate of a shaped body of the first building unit engage the ridges protruding from the base plate of a shaped body of the second building unit stacked on top of said first building unit.
  • the stacked building units each comprise a first and a second shaped body as defined above, and a substrate which does not comprise any magnetocaloric material, said substrate having a first and a second surface opposite to each other, wherein said first surface of said substrate is attached to the second surface of the base plate of said first shaped body and said second surface of said substrate is attached to the second surface of the base plate of said second shaped body.
  • each of the stacked building units consists of a first and a second shaped body as defined above, preferably said shaped bodies each having one or more of the above-defined preferred features, and a substrate, preferably a substrate having one or more of the above-defined preferred features, said substrate having a first and a second surface opposite to each other, wherein said first surface of said substrate is attached to the second surface of the base plate of said first shaped body and said second surface of said substrate is attached to the second surface of the base plate of said second shaped body.
  • the fluid flow structures of adjacent stacked building units are designed so that fitting the ridges of the fluid flow structure of one building unit into the grooves of the fluid flow structure of the adjacent building unit is precluded. This is achieved e.g.
  • the process for manufacturing a magnetocaloric heat exchanger may include assembling of further parts of the magnetocaloric heat exchanger with said heat exchanger block.
  • further parts reference is made to the disclosure provided in the context of the second aspect of the present invention.
  • the process for manufacturing a magnetocaloric heat exchanger as defined above further comprises providing a casing surrounding said heat exchanger block.
  • the heat exchanger block is fixed in the casing by means of a two component (2K) epoxy resin.
  • the particle size of the magnetocaloric material has a D90 value of 5 pm (size distribution analyzed by a Retsch camsizer).
  • the total weight fraction of the particles of said magnetocaloric material is 92.5 % based on the total weight of said particles of said magnetocaloric material and said binding agent.
  • the weight ratio between polyester polyurethane and solvent was about 1 :6.
  • a substrate in the form of an aluminum foil having a thickness of 20 pm was provided.
  • Said mixture was applied to one surface of said substrate by means of slot die coating, thereby forming a coated substrate having a coating layer made up of said mixture dis- posed on said substrate.
  • the coating layer had a thickness of 120 pm.
  • Said coating layer had a first surface facing away from said substrate and opposite to said first surface a second surface in contact with said substrate.
  • Said first surface of said coating layer was treated by means of an embossing roll.
  • the surface of said embossing roll exhibited a structure which is negative with respect to a fluid flow structure comprising a plurality of continuous parallel ridges and a plurality of parallel continuous grooves each extending between two of said ridges, wherein said ridges have a height H of 70 pm and a width W of 50 pm, and said grooves have a width C of 70 pm.
  • Said fluid flow structure does not contain any regions without protruding ridges.
  • Embossing was carried out by means of a calander equipped with a pair of cylindershaped rolls, i.e. an embossing roll acting on the coating layer and a supporting roll supporting the substrate.
  • the embossing roll had a core made of copper and a coating made of hard chromium and was kept at a temperature of about 57 °C.
  • the supporting roll had a hard rubber coating having a thickness of 0.3 mm, and a shore D hardness SH 90. The supporting roll was not heated. Embossing was carried out with a line force of
  • the binding agent was cured by subjecting the coated substrate to a temperature of about 135 °C. During curing the solvent was removed by evaporation. Pieces having lateral dimensions of 2 cm x 1 .5 cm were punched out from the coated substrate. The substrate was not removed from said second surface of said coating layer.
  • a shaped body made up of a mixture comprising a binding agent in the form of a cured polyester polyurethane and particles of a magnetocaloric material having the composition and Curie temperature given above
  • said shaped body comprises
  • a base plate said base plate having a first surface and a second surface opposite to each other
  • a fluid flow structure comprising a plurality of parallel ridges protruding from said base plate and a plurality of grooves each extending between two of said ridges
  • said base plate has a base plate thickness B of 90 pm
  • said ridges have a height H of 70 pm
  • said ridges have a width W of 50 pm, measured at half of height H
  • Said fluid flow structure does not contain any regions without protruding ridges.
  • the cross section of the grooves and ridges exhibited some deviation from a rectangular shape, i.e. the corners were slightly rounded.
  • H/B 0.77
  • H/C 1
  • H/W 1.4.
  • Said grooves allow for the flow of a heat transfer fluid.
  • a heat exchanger block was obtained consisting of 100 building units as described above, wherein in each case between two building units stacked one on top of the other the ridges protruding from the base plate of the shaped body of the first building unit engage the substrate attached to the base plate of the shaped body of the second building unit stacked on top of said first building unit, so that the ridges protruding from the base plate of the shaped body of the first building unit and the substrate attached to the base plate of the shaped body of the second building unit stacked on top of said first building unit cooperate to define channels for the flow of a heat transfer fluid.
  • the heat exchanger block has a total height of about 2 cm.
  • the heat exchanger block was sur- rounded by an encasing made of glass-fiber reinforced plastic. In said encasing the heat exchanger block was fixed by means of a two component (2K) epoxy resin.

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Abstract

L'invention concerne des unités de construction pour un bloc d'échangeur de chaleur pour un échangeur de chaleur magnétocalorique, des échangeurs de chaleur magnétocaloriques comprenant un bloc d'échangeur de chaleur comprenant au moins deux desdites unités de construction, ainsi que des procédés de fabrication desdites unités de construction et desdits échangeurs de chaleur magnétocaloriques.
PCT/EP2018/085629 2017-12-18 2018-12-18 Unité de construction pour échangeur de chaleur magnétocalorique WO2019121766A1 (fr)

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EP17208106 2017-12-18
EP17208106.9 2017-12-18

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WO2019121766A1 true WO2019121766A1 (fr) 2019-06-27

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US20140020881A1 (en) 2007-12-27 2014-01-23 Vacuumschmeize GmbH & Co. KG Composite article with magnetocalorically active material and method for its production
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