CN102660229B - Incombustible mixed refrigerant suitable for copious cooling temperature of 90-140DEG C below zero - Google Patents
Incombustible mixed refrigerant suitable for copious cooling temperature of 90-140DEG C below zero Download PDFInfo
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Abstract
The invention relates to an incombustible mixed refrigerant suitable for the copious cooling temperature of 90-140DEG C below zero, which comprises the following five groups of substances: the first group is nitrogen, argon, methane or mixture; the second group is R14; the third group is R23, R116, R170, R1150, R41 or mixture; the fourth group is R218, R125, R32, R143a, R290, R1270, R13I1, R134, R134a, R152a, R1216 or mixture; the fifth group is R1234ze, R245cb, R227ea, R3110, R236fa, R254cb, R143, R236ea, R245fa, R329mcc, R347mcc, R338mcf, R245eb, R245ca, R338mee, R338mcc or mixture; the molar concentrations of the five groups are respectively 5-35%, 10-40%, 5-20%, 5-20% and 5-25%. The incombustible mixed refrigerant suitable for the copious cooling temperature of 90-140DEG C below zero has the advantages of low integral greenhouse effect, no ozone damage and the like, is safe in a regeneration type throttling and refrigerating system, and refrigeration in the temperature zone of 90-140DEG C below zero can be realized.
Description
Technical field
The present invention relates to the refrigeration agent in refrigeration and low temperature technique field, the particularly non-combustible mix refrigerant of a kind of being suitable for-90～-140 ℃ cryogenic temperature, this Diversity refrigeration agent is efficient, safety environmental protection.
Background technology
Utilize the Cryogenic mixed-refrigerants j-t refrigerator of backheat measure to have efficiently, the advantage such as reliable and low cost of manufacture, be widely used in the energy, chemical industry and cryogenic engineering field, for realizing the aspects such as liquefaction of the cooling and industrial gasses of device depth, fields such as cryogenic refrigerator, natural gas liquefaction.Except the hardware facilities such as refrigeration system flow process and compressor and interchanger, what this Refrigeration Technique was the most key is Diversity refrigeration agent.Be applied to the Diversity refrigeration agent of mixed work medium for throttling refrigeration system according to requirement and the system structure design of refrigeration warm area, conventionally require 3～7 kinds of constituent elements to form, show as typical non-azeotropic feature, and utilize the temperature variant nonlinear characteristic of enthalpy between its phase change zone, realize the thermal equivalent coupling between high-low pressure refrigeration agent, thereby improve refrigerating efficiency.From another one angle, set forth, the temperature range that each constituent element undergoes phase transition at it has higher isothermal throttling effect, and each constituent element with different boiling temperature is according to the relay of boiling point High-low Match, can forms mix refrigerant and across scope, there is higher refrigeration effect in whole refrigeration temperature.About refrigeration agent screening and thermodynamic optimization principle can, referring to relevant academic documents, repeat no more here.
Owing to being subject to the Basic Physical Properties parameter limit such as boiling point, freezing point temperature of constituent element, also have in addition other physicochemical property such as combustibility, toxicity of constituent element working medium, the optional constituent element under the effective constituent element of mixing medium, especially low temperature is very limited.At present by some mandates or apply for a patent and relate to deep cooling mixing medium and form and concentration proportioning, wherein granted patent ZL 97115295.0, ZL 03121423.1,03121466.5 minute warm area of ZL 03121467.3 and ZL has proposed the serial multicomponent mixture work medium for copious cooling throttle Refrigeration Technique, wherein constituent element has the fluorochemical of nitrogen, alkane and part alkane to form, mixture ozone free damage effect.Each constituent element of mixture is divided into cold zone constituent element, the normal warm area constituent element that freezes according to boiling point difference, middle high-temperature zone constituent element and high-temperature zone constituent element, and each warm area constituent element, according to the multicomponent mixture work medium of a concentration ratio acquiring demand, has higher thermodynamic(al) efficiency.The alkanes substances such as the methane wherein containing, ethane and propane have the mutual solubility good with lubricating oil, and Greenhouse effect are little, and environmental protection characteristic is good, but it is certain flammable to cause system to exist.And due to the existence of combustiblecomponents, make system all need to consider the measures such as explosion-proof in links such as production, debugging, maintenance and use occasions, increased the difficulty that production cost and user accept.
There is ZL 01802606.0 (publication number: CN 1388887A, similar content appears in the middle of US6502410 patent with it) hydrofluoride (HFCs) and perfluoro-compound (FC) with nitrogen (N2), argon gas (Ar) and alkane proposed, the non-combustible Diversity refrigeration agent forming such as R23, R125, R134a, R236fa and R245fa etc., wherein minimum temperature can realize 105K, also contains the compositions such as neon (Ne), helium (He).This patent is different according to refrigeration warm area equally, for the constituent element in mixture, according to its boiling point, is divided into different zones, by each warm area different boiling constituent element, according to finite concentration proportional range, forms whole mixt.Its whole mixture is not containing flammable alkanes composition, and also not hydrogeneous fluorochlorohydrocarbon (HCFC) class has the component of ozone layer destroying.It is poor that but its efficiency contains the mixture of alkane.Wherein in order to adopt, avoid flammable, its non-combustible HFC class material of choosing all has the higher Greenhouse effect value (GWP) of diving as high boiling point constituent elements such as HFC125, HFC236fa.
Separately there is US Patent No. 5408848 to propose a kind of employing and do not contain the mixing medium Refrigeration Technique of CFC constituent element,-150 minimum to meet ℃ above refrigeration demand, has wherein provided in an embodiment and take R142b, R134a, R23, R14 and Ar as main mixing medium composition.In this compositions of mixtures, not containing combustibleconstituents, still wherein containing R142b is HCFC material, has depletion of the ozone layer effect, belongs to the row of restriction and forbidding.
When adopting mixed work medium for throttling Refrigeration Technique to realize the situation of deep refrigerating, according to deep cooling mixing medium Refrigeration Technique principle, the boiling point of the required constituent element of multicomponent mixture work medium that it adopts should be according to refrigeration warm area, (concrete elaboration seen Cryogenics by minimum temperature (should lower than or at least equal lowest refrigerating temperature), to start to be increased to gradually envrionment temperature, Volume 44, Issue 12, and December 2004, Pages 847-857).Therefore realize cryogenic refrigeration, for example, in the time of-140 ℃, in mixture, must have boiling point to exist lower than the constituent element of-140 ℃, for example Ar or N2.Due to the lower boiling constituent element limited amount that nature exists, in natural medium, non-flammable material, generally by materials such as He, Ne, N2, Ar, only has R14 etc. in the middle of synthetic material.To realize cryogenic refrigeration in addition, except the boiling point of material is applicable to, also need freezing point temperature enough low, to avoid separating out at low temperatures solid, stop up fluid channel, especially throttle capillary tube.Therefore when realizing cryogenic refrigeration, in the constituent element of minimum warm area, the materials such as He, Ne, N2, Ar and R14 are essential according to the refrigeration warm area that will realize substantially, especially the material such as N2, Ar, R14 and R23.This also can find out from patent ZL 01802606.0 and US5408848, these two patents have all comprised the materials such as N2, Ar, R14 and R23, but in the mixture of its composition, also contain different composition, for example US5408848 has R142b, and ZL 01802606.0 contains the materials such as R125, R245fa and R236fa.
As everyone knows, for a kind of mixture being formed by many kinds of substance, its hot physical property is determined by mixture constituent element and constituent element concentration, wherein but the identical concentration of the difference of constituent element or constituent element is different, all can form diverse mixture, this hot physical property such as equivalent weight, critical parameter, enthalpy entropy that shows mixture is all variant.Constituent element is identical and concentration difference shows more in general cold mixt refrigeration agent, the zeotrope for example being formed by R32, R125 and tri-kinds of materials of R134a, owing to forming the difference of concentration, can be divided into different refrigeration agents, its application scenario is also not quite similar, the mixture and the business-like numbering that above-mentioned three kinds of materials, consist of at present can specifically be divided into the refrigeration agents such as R407A～R407E, and it has diverse physical property and alternative object.These are set forth and analyze is just a problem of explanation, and by comprising the even identical constituent element of part same components, different concns can form diverse mixture, and it specifically can be determined by corresponding target.
According to above-mentioned analysis, can know in the middle of prior art and realize and comprised the polynary non-combustible mix refrigerant of deep cooling being formed by N2, Ar, R14, R23 and other high boiling substances etc., but in the middle of this type of mix refrigerant in high boiling point constituent element or adopted R142b etc. to contain the dive material of value (ODP) of ozone layer destroying, adopted R236fa etc. to have the hydrogen fluorohydrocarbon material of high-temperature chamber effect (GWP), these all make its environmental protection characteristic be affected.In addition, the mutual solubility of most HFC and FC class material and lubricating oil is poor, there is in addition the HFC of higher and the freezing point temperature of FC class material is all higher, and the molten oiliness of the low temperature of its mix refrigerant is poor, therefore above-mentioned non-combustible mix refrigerant is generally applied in the middle of multistage automatic cascade refrigeration system.In the middle of adopted system, multistage vapor-liquid separating device is set conventionally, lubricating oil and the constituent element with high-solidification point temperature are separated in higher temperatures district, with assurance system, normally to work, this has obviously increased the complicacy of system.
In addition, research is found: 1. some non-flammable high boiling point working medium have certain dissolving power in the low boiling working fluid that can Gong select, by component controls with working medium to selection can effectively avoid high boiling point component at low temperatures solidify obstructing problem; 2. in multicomponent mixture, both just contained comhustible component, as long as choose other component and control the concentration of comhustible component, it is non-flammable or within safety range can making equally multicomponent mixture.Based on above-mentioned cognition, the present invention proposes efficient, safety and the environmental protection Diversity refrigeration agent of a kind of being applicable to-90～-140 ℃ cryogenic temperature.
Summary of the invention
The object of the invention is to: take into account the characteristics such as efficient, the safety of deep cooling mixing medium and environmental protection, and provide a kind of and be suitable for the non-combustible mix refrigerant of-90～-140 ℃ of cryogenic temperatures, this mix refrigerant is efficient, also environmental protection of safety, can be applicable in back-heating type mixed work medium for throttling refrigeration system to realize the refrigeration of-90～-140 ℃ of warm areas.
Technical scheme of the present invention is as follows:
The non-combustible mix refrigerant of provided by the invention being suitable for-90～-140 ℃ cryogenic temperature, it is comprised of following five groups of materials, and these five groups of materials are respectively:
First group of material is nitrogen (N
2), argon (Ar), methane (CH
4) or the mixture of any two materials compositions wherein or the mixtures of three kinds of material compositions;
Second group of material is tetrafluoromethane (CF
4, R14);
The 3rd group of material is trifluoromethane (CHF
3, R23), hexafluoroethane (CF
3cF
3, R116), ethane (C
2h
6, R170), ethene (C
2h
4, R1150), a fluoromethane (CH
3f, R41) or the mixture of any two materials compositions wherein or the mixture that many kinds of substance wherein forms;
The 4th group of material is perfluoropropane (C
3f
8, R218), pentafluoride ethane (CHF
2cF
3, R125), methylene fluoride (CH
2f
2, R32), Halothane (CH
3cF
3, R143a), propane (C
3h
8, R290), propylene (C
3h
6, R1270), CF3I (CF
3i, R13I1), 1,1,2,2-Tetrafluoroethane (CHF
2cHF
2, R134), HFA 134a (CH
2fCF
3, R134a), 1,1-C2H4F2 C2H4F2 (CH
3cHF
2, R152a), the mixture that forms of the mixture that forms of R 1216 (CF2=CFCF3, R1216) or any two materials wherein or many kinds of substance wherein;
The 5th group of material is 1,3,3,3-tetrafluoeopropene (CF
3cH=CHF, R1234ze), 1,1,1,2,2-pentafluoropropane (CH
3cF
2cF
3, R245cb), HFC-227ea (CF
3cHFCF
3, R227ea), perfluorinated butane (C
4f
10, R3110), 1,1,1,3,3,3-HFC-236fa (CF
3cH
2cF
3, R236fa), 1,1,2,2-tetrafluoropropane (CH
3cF
2cHF
2, R254cb), Halothane (CH
2fCHF
2, R143), 1,1,1,2,3,3-HFC-236fa (CHF
2cHFCF
3, R236ea), 1,1,1,3,3-pentafluoropropane (CHF
2cH
2cF
3, R245fa), 1,1,1,2,2,3,3,4,4-nine fluorine butane (CHF
2cF
2cF
2cF
3, R329mcc), 1,1,1,2,2,3,3-seven fluorine butane (CH
3cF
2cF
2cF
3, R347mcc), 1,1,1,2,2,4,4,4-Octafluorobutane (CF
3cH
2cF
2cF
3, R338mcf), 1,1,1,2,3-pentafluoropropane (CH
2fCHFCF
3, R245eb), 1,1,2,2,3-pentafluoropropane (CH
2fCF
2cHF
2, R245ca), 1,1,1,2,3,4,4,4-Octafluorobutane (CF
3cHFCHFCF
3, R338mee), 1,1,1,2,2,3,3,4-Octafluorobutane (CH
2fCF
2cF
2cF
3, the mixture that the mixture that any two materials R338mcc) or wherein form or many kinds of substance wherein form;
The volumetric molar concentration sum of respectively organizing material in the mixture that described five groups of materials form is 100%;
Wherein, the volumetric molar concentration of described first group of material is 5%～35%;
The volumetric molar concentration of described second group of material is 10%～40%;
The volumetric molar concentration of described the 3rd group of material is 10%～30%;
The volumetric molar concentration of described the 4th group of material is 5%～20%;
The volumetric molar concentration of described the 5th group of material is 10%～25%.
The non-combustible mix refrigerant of of the present invention being suitable for-90～-140 ℃ cryogenic temperature, when first group of material selected methane, volumetric molar concentration≤25% of methane in described mix refrigerant.
The non-combustible mix refrigerant of of the present invention being suitable for-90～-140 ℃ cryogenic temperature, when the 3rd group of material selected the mixture of ethane, ethene, a fluoromethane or any two materials compositions wherein or the mixture that three kinds of materials wherein form, volumetric molar concentration≤25% of described the 3rd group of material in described mix refrigerant.
The non-combustible mix refrigerant of of the present invention being suitable for-90～-140 ℃ cryogenic temperature, when the 4th group of material selected methylene fluoride, Halothane, propane, propylene, 1, the mixture that the mixture that 1-C2H4F2 C2H4F2 or any two materials wherein form or many kinds of substance wherein form, volumetric molar concentration≤20% of described the 4th group of material in described mix refrigerant.
The non-combustible mix refrigerant of of the present invention being suitable for-90～-140 ℃ cryogenic temperature, at the methane of the first component; In the methylene fluoride of the ethane of the 3rd component, ethene and a fluoromethane and the 4th component, Halothane, propane, propylene and 1,1-C2H4F2 C2H4F2, while selecting two kinds of materials or many kinds of substance simultaneously, their volumetric molar concentration sum≤25%.
Above-mentioned mix refrigerant concentration range exists corresponding to working pressure range: high pressure is in 1.6～2.3MPa scope, and low pressure (is absolute pressure) within the scope of 02～0.6MPa, and normal pressure ratio scope is between 3～10.Wherein the change in concentration general trend of constituent element is to increase with low pressure, and lower boiling constituent element concentration increases, and corresponding middle high boiling point constituent element concentration reduces, and vice versa.Adopt the back-heating type mixed work medium for throttling refrigeration system of above-mentioned mix refrigerant can take in higher temperatures district one-level vapour liquid separator, make the separated backflow of lubricating oil and part high boiling point constituent element, guarantee security of system reliability service, concrete refrigeration cycle structure can be referring to public technologies such as patent ZL00136709.9, or other similar cycle structures, repeat no more here.
Adopt the regenerative refrigerating system of above-mentioned mix refrigerant can realize safely, efficiently-90～-140 ℃ of warm area refrigeration, compare with existing deep cooling mix refrigerant, it has complete non-inflammability or only weak flammable, and whole Greenhouse effect are low, non ozone depleting effect, has significant advantage completely.
Embodiment
Embodiment 1-3
Preparation the present invention runs on the complete non-combustible of-90 ℃ of warm areas or weak flammable Diversity refrigeration agent only, and the minimum heat transfer temperature difference in interchanger inside is 1K, and envrionment temperature is 35 ℃, and its Diversity refrigeration agent working medium concentration and performance see the following form:
Embodiment 2: preparation runs on the complete non-combustible of-110 ℃ of warm areas or weak flammable Diversity refrigeration agent only, and the minimum heat transfer temperature difference in interchanger inside is 1K, and envrionment temperature is 35 ℃, and its Diversity refrigeration agent working medium concentration and performance see the following form:
Embodiment 3: preparation runs on the complete non-combustible of-140 ℃ of warm areas or weak flammable Diversity refrigeration agent only, and the minimum heat transfer temperature difference in interchanger inside is 1K, and envrionment temperature is 35 ℃, and its Diversity refrigeration agent working medium concentration and performance see the following form:
In above-described embodiment, the regenerative refrigerating system complete non-combustible or only weak flammable mix refrigerant adopting can realize-90～-140 ℃ of warm area refrigeration safely, efficiently, compare with existing deep cooling mix refrigerant, it has complete non-inflammability or only weak flammable, and whole Greenhouse effect are low, non ozone depleting effect, has significant advantage completely.
Claims (4)
1. non-combustible mix refrigerant, in an application for-90～-140 ℃ of deep cooling warm areas, is characterized in that, described non-combustible mix refrigerant is comprised of following five groups of materials, and these five groups of materials are respectively:
First group of material is N
2, Ar, methane or any two materials wherein mixture or the three kinds of mixtures that material forms that form;
Second group of material is tetrafluoromethane;
The 3rd group of material is trifluoromethane, hexafluoroethane, ethane, ethene, a fluoromethane or the mixture of any two materials compositions wherein or the mixture of the composition of many kinds of substance wherein;
The 4th group of material is pentafluoride ethane, methylene fluoride, CF3I, 1,1,2, the mixture that two kinds of materials in 2-Tetrafluoroethane, HFA 134a, R 1216 or these materials or many kinds of substance form;
The 5th group of material is 1, 3, 3, 3-tetrafluoeopropene, 1, 1, 1, 2, 2-pentafluoropropane, 1, 1, 1, 2, 3, 3, 3-heptafluoro-propane, 1, 1, 1, 3, 3, 3-HFC-236fa, 1, 1, 2, 2-tetrafluoropropane, 1, 1, 1, 2, 3, 3-HFC-236fa, 1, 1, 1, 3, 3-pentafluoropropane, 1, 1, 1, 2, 2, 3, 3, 4, 4-nine fluorine butane, 1, 1, 1, 2, 2, 3, 3-seven fluorine butane, 1, 1, 1, 2, 2, 4, 4, 4-Octafluorobutane, 1, 1, 1, 2, 3-pentafluoropropane, 1, 1, 2, 2, 3-pentafluoropropane, 1, 1, 1, 2, 3, 4, 4, 4-Octafluorobutane, 1, 1, 1, 2, 2, 3, 3, the mixture that the mixture that 4-Octafluorobutane or any two materials wherein form or many kinds of substance wherein form,
The volumetric molar concentration sum of respectively organizing material in the mixture that described five groups of materials form is 100%;
Wherein, the volumetric molar concentration of described first group of material is 5%～35%;
The volumetric molar concentration of described second group of material is 10%～40%;
The volumetric molar concentration of described the 3rd group of material is 10%～30%;
The volumetric molar concentration of described the 4th group of material is 5%～20%;
The volumetric molar concentration of described the 5th group of material is 10%～25%.
2. the application at-90～-140 ℃ of deep cooling warm areas by non-combustible mix refrigerant claimed in claim 1, is characterized in that: in described first group of material, select methane, volumetric molar concentration≤25% of methane in described mix refrigerant.
3. the application at-90～-140 ℃ of deep cooling warm areas by non-combustible mix refrigerant claimed in claim 1, it is characterized in that: described the 3rd group of material selected the mixture of ethane, ethene, a fluoromethane or any two materials compositions wherein or the mixture that three kinds of materials wherein form, volumetric molar concentration≤25% of described the 3rd group of material in described non-combustible mix refrigerant.
4. the application at-90～-140 ℃ of deep cooling warm areas by non-combustible mix refrigerant claimed in claim 1, it is characterized in that: in described methane, ethane, ethene, a fluoromethane and methylene fluoride, while selecting two kinds of materials wherein or many kinds of substance simultaneously, their volumetric molar concentration sum≤25%.
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| CN201210127046.0A CN102660229B (en) | 2012-04-26 | 2012-04-26 | Incombustible mixed refrigerant suitable for copious cooling temperature of 90-140DEG C below zero |
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| CN115433545A (en) * | 2022-09-28 | 2022-12-06 | 安徽中科都菱商用电器股份有限公司 | Novel environment-friendly mixed refrigerant |
| CN115975602B (en) * | 2023-03-17 | 2023-06-30 | 北京星宇环试科技有限公司 | Non-combustible mixed refrigerant suitable for low-temperature system |
| CN116606632B (en) * | 2023-07-19 | 2023-10-20 | 中科美菱低温科技股份有限公司 | Refrigerant and method for producing the same |
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Application publication date: 20120912 Assignee: Zhongke Keling (Beijing) Technology Co.,Ltd. Assignor: CHINA-SCICOOLING (BEIJING) SCIENCE & TECHNOLOGY CO.,LTD. Contract record no.: X2022990000338 Denomination of invention: Non combustible mixed refrigerant suitable for cryogenic temperature of -90~-140 degC Granted publication date: 20140507 License type: Common License Record date: 20220701 |