CA1052685A - Removal of mass or energy from a gas in a packed column with fibrous bed - Google Patents
Removal of mass or energy from a gas in a packed column with fibrous bedInfo
- Publication number
- CA1052685A CA1052685A CA223,176A CA223176A CA1052685A CA 1052685 A CA1052685 A CA 1052685A CA 223176 A CA223176 A CA 223176A CA 1052685 A CA1052685 A CA 1052685A
- Authority
- CA
- Canada
- Prior art keywords
- bed
- liquid
- gas
- fibers
- bodies
- Prior art date
- Legal status (The legal status 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 status listed.)
- Expired
Links
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/30—Loose or shaped packing elements, e.g. Raschig rings or Berl saddles, for pouring into the apparatus for mass or heat transfer
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D47/00—Separating dispersed particles from gases, air or vapours by liquid as separating agent
- B01D47/14—Packed scrubbers
-
- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F28—HEAT EXCHANGE IN GENERAL
- F28F—DETAILS OF HEAT-EXCHANGE AND HEAT-TRANSFER APPARATUS, OF GENERAL APPLICATION
- F28F25/00—Component parts of trickle coolers
- F28F25/02—Component parts of trickle coolers for distributing, circulating, and accumulating liquid
- F28F25/08—Splashing boards or grids, e.g. for converting liquid sprays into liquid films; Elements or beds for increasing the area of the contact surface
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/30—Details relating to random packing elements
- B01J2219/302—Basic shape of the elements
- B01J2219/30269—Brush
Landscapes
- Chemical & Material Sciences (AREA)
- Physics & Mathematics (AREA)
- Thermal Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Engineering & Computer Science (AREA)
- Organic Chemistry (AREA)
- Mechanical Engineering (AREA)
- General Engineering & Computer Science (AREA)
- Vaporization, Distillation, Condensation, Sublimation, And Cold Traps (AREA)
- Physical Or Chemical Processes And Apparatus (AREA)
- Gas Separation By Absorption (AREA)
Abstract
ABSTRACT OF THE DISCLOSURE
A packed column for mass and/or heat transfer including a bed of bodies of fibrous material. Each body is of generally cylindrical form and includes a centrally disposed axial support from which a large number of crimped fibers extend, the fibers being secured to the support. The bodies are disposed in the bed at random and interlock with each other.
The density of the fibers in count per unit volume of bed varies from point to point in the packing body and in the bed.
The volume of each body is small compared to the volume of the column. A liquid is distributed over the top of the column and trickles downwardly through the packing in a multitude of irregula?
paths while the gas is projected upwardly through the packing.
The gas contacts the liquid over a very large surface area for an extended time interval and effective mass and/or heat transfer between the gas and liquid takes place.
A packed column for mass and/or heat transfer including a bed of bodies of fibrous material. Each body is of generally cylindrical form and includes a centrally disposed axial support from which a large number of crimped fibers extend, the fibers being secured to the support. The bodies are disposed in the bed at random and interlock with each other.
The density of the fibers in count per unit volume of bed varies from point to point in the packing body and in the bed.
The volume of each body is small compared to the volume of the column. A liquid is distributed over the top of the column and trickles downwardly through the packing in a multitude of irregula?
paths while the gas is projected upwardly through the packing.
The gas contacts the liquid over a very large surface area for an extended time interval and effective mass and/or heat transfer between the gas and liquid takes place.
Description
BAC~CGROUMD OF THE INVENTION
-This invention relates to mass and/or heat transfer and has particular relationship to mass or heat transfer taking place between counterflowing fluids through packing. ~ass-transfer operations such as gas scrubbing, distillation and the like are carried out by counterflow of a gas and a liquid between which the mass transfer is to take place through a medium whose purpose is to maximize the contact surface or area between the gas and liquid without blocking the gas flow altogether by so-called flooding. Flooding is defined as the limiting. condition which occurs when, as gas or liquid flows are increased, the gas phase becomes discontinuous, the gas-pressure drop becomes unstable, and the bed tends to fill with liquid. Common types of prior-art * *
packing materials include such bodies as Raschig rings and Berl . * Trade Mark . ~
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lO~;~S85 1 and Intalox saddles as disclosed in U.S. Leva patent 2,639,909.
These common packings are effective as liquid dispersal surfaces but have the disadvantage of relatively high gas-flow resistance and a susceptibility to flooding at relatively low rates of gas and liquid flow. Design fluid-~low capacities of packed towers are based principall~ on two criteria: the flood limit and the intrinsic gas-flow resistance of the packing. (B.J.Lerner and C.S.Grove, Jr. - Industrial and Engineering Chemistry Vol. 43, pgs. 216-225 Jan. 1951). A consequent disadvantage of such conventional packings in the smaller sizes is the need for un-economically large tower-shell diameter required to keep the gas velocity below the flooding point or to keep gas flow resistance ;
and dependent blower costs within economic limits.
In recent years, commercial packed-tower design practice has been directed toward obtaining higher gas velocities, or low gas flow resistance, and thus more econo~ic smaller tower-shell diameters. Typical of the teachings of the prior-art attempts to ~` meèt this objective are the following U.S.patents:
~ Kleinschmidt 2,143,016 - Smucker 2,607,714 Dixon 2,615,832 - Teller 2,867,425 ~eeping 2,921,776 - Robjohns 3,293,174 Lerner 3,410,057 Lipins~i 3,438,614 ~ These patents disclose beds of randomly disposed packing materials ,` for extending the surface contact between the phases taking part ~`; in the mass transfer. Lower gas-flow resistances and higher gas-; -. .
flow velocities have been achieved through the use of larger sizes of convenkional tower packings such as saddles, and the use of , more "open" distributed-surface packings such as Pall rings and ,., ~ .
~,,, *
Tellerettes (Teller), which flood at much higher liquid and gas ~ flow rates than do the older types of packings. However, in the ... .
,, * Trade Mark : !
r,~
lOS~;85 use of mass tran~fe~ oolumns including paoking o~ this prior-art type there has been experienced the emission o~ liquid spray in large quantities from the top of the ¢olumns, which militates against transfer e~ioiency.
It is an ob~ect of this invention to provide high-oapaoity, high~e~iciency mass~trans~er paoked columns or to~ers whioh sh~ll transmit the gas at relatively high velocities, without exoessive gas-flow resistanoe, shall not ~lood until the liquid and gas-flow rates reach relatively high magnitudes, and ~; 10 shall not em~t spray in large quantities from the top o~ the ; oolumns.
Summa~Y 0~ The Invention It has been discovered from tests o~ the prior-art high-flow-rated beds o~ high-Ilood-point packing structures that theg deYelop a mode o~ ~ailuxe not enco~ntered beiore, ahead o~ the flood point. As gas or li~uid flow is incxeased, beds of these paokings fail first not by ~looding, but by severe spxay or entrainment carxyover. Spray carxyover is the trans~er o~ the liquid in droplets to the gas and the concurrent movement of these droplets by the gas. In most cases, spxay or entrainment oarryover with the gas-ana-liquid system begins in these packings a~ approximately 4 to 6 ~eet per second superfi¢ial gas velocity (based on ~ree tower ¢ross-se¢tional area; i.e., disregarding the volume oc¢upied by the pa¢king) at nom~n~l liquid irrigation rates, and in the absen¢e o~ an ei~icient mist eliminator above the bed, reaches inoperable carryover rates at about 6-8 feet ;~ per second super~ioial gas velo¢ities~
At ga5 velo¢ities greater than 4 to 6 feet per se¢ond for gas densities similar to air at standard atmospheric ¢onditions, liquld tends to be stripped o~ ~n egtended planar sur~a¢e in drop ~ form by gas ~ri¢tion. ~he size o~ liquid drops that can be - supported in an upward-flowing gas stream oan be oalculated b~
. , .
~ 05;~;85 Stokes' law~ but in genexal, the fine~ droplets a~e suppo~ted at the low gas velooities, while la~ge~ and heavie~ drops aYe ent~ained at the highe~ gas velo¢ities. Thus, it has been disoove~ed that in addition to the sp~ay from the top of the ; bed o~ column obseYved with high-velocity ¢onventional paokings, which amountis to a substantial fxa¢tion o~ the liquid input at gas velocities in ex¢ess o~ 5 to 6 feet per se¢ond, thexe is also the isame high degree of baok-sp~ay within the inteYnal voids o~ the packing. ~his inte~nal xeci~oulation of liquid within - 10 a paoked bed employed fo~ oounte~cur~ent gas-liquid oontaoting oausesi depa~tuxe fxom t~ue ¢ounte~ou~ent flow, impai~-s the trans~e~ effi¢iency, and is highly undesixable.
It is an object of this invention to eliminate oY
supp~ess this eife¢t and to p~ovide a packing whiah, by YeaSon oe its gene~al intrinsi¢ st~uotu~e, behaves as an e~i¢ient mist eliminato~, has eiieotive liquid-dispexsal p~ope~ties and yet pYesents to the gas a minimum o~ extended planar su~faoes ~xom . .
which the liquid can be entrained. ;
;. .
~ It has been ~ealized in a~iving at this invention that : -, what is desi~able is packing whose density varies f~om point to point in the bed so as to achieve effective ~adial dispe~sion o~
the liquidO ~he prio~-axt packing does not e~ieotively meet this condition.
Wi~e mesh packings, such as those di~closed by Di~on ;., ~j ~- and Keeping, have uni~o~m capillaYy p~ope~ties, and behave like .,-1 .
:` solid-wall packings when wet. Not only is liquid ~eadily ~e-i~ ent~ained f~om these packings, but these packings are not liquid-dispexsing and they do not se~ve ais e~ficient mist eliminators.
Non-capilla~y fibrous-pellet packings su¢h as those o~ ~exne~
~0 have desirable p~ope~ties; they aYe e~fi¢ient inte~nal mist eliminatoYs. Howeve~, the low and fairly unifoYm spatial density ;' ,:
., ~
~.o5;~85 1 f fibers giving the necessary non-capillarity, yields low liquid retention and causes the liquid at times to channel directly through the packing, so that these packings have low mass-transfer characteristics. Similarly, fiberglass mats, such as those described in Xleinschmidt, suffer from liquid channelling behavior, and are essentially non-dispersive for liquids, giving inferior countercurrent-contact transfer per-formance as compared to planar packings.
In accordance with this invention a new type of packing is provided which has been found to have unique liquid-dispersion properties for effecting gas-liquid contact, and which allows high gas-velocity-low-pressure-drop operation while providing for internal mist elimination. This invention is a mass-transfer or heat-transfer column or tower operating by counter-flow of a gas and liquid having a bed of fibrous bodies or packing elements formed of a multitude of fibers extending radially from a central axial support ~o which the fibers are secured. ~he dimension of the bodies is small relative to the dimension of the column~
Typically the bodies are regularly-shaped, for example of circularly cylindrical form with the height substantially equal to the diameter. The minimum dimension of the column is typically ei~ht to ten times the diameter of a packing~body and the minimum depth of the bed about three times the diameter of the packing ~ body. Typical columns may have a diameter as small as one foot ; and as large as twenty-five feet. The diameter of a packing body should be so related to the density of the radial fibers extending from the axial support that the density of the fibers, in counts per unit volume of the region of fibers, at the periphery of the body is about one-half thedensity or less near the axis of the body.
This invention achieves an important desideration, namely a non-uniform distribution or density of the fibers, in :'~
~0~ 85 I counts per unit volume of the bed from region to region throughout the bed. While this desideration is achieved in a unique and highly advantageous manner with the radial bodies or elements, other modes of achieving this desideration are within the scope of this invention.
In the usual practice of this invention the bodies or elements are randomly disposed in the column with their fibers interlocked. The diameter and/or height of the packing body is large compared to the diameter of the fibers. Typically O the packing body diameter and height are 2 to 4 inches and the diameter of a fiber is .010 to .020 inch. The fibers should be ..
sufficiently strong to resist substantial deformation under the loads impressed on the fibers during mass-transfer operation.
A random bed of fibrous bodies in accordance with this i invention forms an interlocking three-dimensional extended-surface packing with a mar~ed degree of non-uniform spatial density, yielding excellent liquid-dispersion properties, low gas flow resistance, excellent mist elimination characteristics and unique mass-transfer properties. The packing body is very light in .; .
weight and can be made from low-cost, corrosion-resistant ' materials. It is characterized by very high gross void space and very low pressure drops even at high rates of gas and liquid flow. It is highly resistant to both flooding and to internal ~ and external spray carryover.
; A unique feature of the packing in accordance with this ` ~ invention is the variable spatial fiber density of the element, which imparts outstanding advantages over prior-art mesh or fiber . ~
packing elements. The relatively high density of fibers in the axial region around the stem or core of the element causes any , . ~ 30 impinging liquid stream to be intercepted, deflected, dispersed and spread out, generally in the form of multiple smaller li~uid ' ~
105;~685 streams or droplets dixected radial~y away fxom the stem along the ~ibexs. ~his spxeading action ~s independent of the orienta-tion of the element in the bed~ so that the bed is not only highly xesistant to liquid channeling, but achieves a unigue deg~ee o~
xadial dispexsion and re-dispexsion of the liquid.
Depending on the natuxe of the liquid-gas contacting operation, it may be desirable to utilize ~ ~*~si ~hat are either non-wettable or wettable by the liquid phase. ~ox e~ample, in cextain ope~ations, where diffusion xesistanoe within the liquid phase oontxols of~mass txansfex and liquid mixing is desirable ox essential, it is pxefexable to utilize non-wetting fibers so that liquid drops roll along the fibers. ~he rolling o~ the dxops has a stixring action Nhioh enhances the diffusion of the trans-ferxed matter on the surfaoe of the drops throughout the dxops.
Alternately, in certain cases of absorption o~ desorption of a gas ¢omponent to or from the liquid phase (whexe gas diffusion oontxols), it may be desixable to use fibers that are wettable by the liquid, 90 that the liquid is transferxed along the fiber surfaoes as a ¢ontinuous high-sux~a¢e-area thin film. In both ¢ases, non-wettable and wettable fibers, the radial transfer meohanism sexves to transfex liquid fxom the stem xegion to the outer low-iibe~-density xegion of the element whexe the gas pre-domlnately tends to flow be¢ause of the lowe~ flow xesistanoe~
~hus, the unique liquid dispersion me¢hanism sexves to ¢ontinuously txansfeY liquid ~xom regions whexe it would be xelati~ely shielded ~rom buIk-gas-~low ¢ontact to xe~ions whexe the major poxtion of ~; the gas tends te flow. ~uxther, a portion of the fibrous element intexlooks with the peripheral fibexs of its neighboxs, thus allowing the trans~er of liquid from body to body dixe¢tly along ~0 the in~exlocking fibexs. ~iquid that does not txansfex along inte~locking fibers, "dead-ends" at the end of the fiber, and ' .
~05;~685 1 forms drops which then fall through the interstitial space, thus contributing to liquid mixing and redistribution. In the prior-art solid or mesh-surface packings, the free-fall distance of such drops is relatively long, of the order or magnitude of one or more packing diameters, and relatively little mass transfer takes place during this free-fall distance because of the tendency to surface stagnation of small drops. In the fibrous-body bed according to this invention, the free-fall drop distance is a small fraction of the packing diameter because the fibers occupy `
most of the volume of the bed and fiber-to-fiber distances are small. Further, the fibrous packing has a uniquely very large . ~ -number of fiber ends at which free-fall drops are generated.
Gas mixing, which is secured in a prior-art packed bed composed ~-of planar solid bodies by turbulent flow through non-uniform free void volume, is obtained in`the case of the radial fiber-eiement bed according~to this invention by gas flow through volumes , of varying fiber count in the bed or volume density. The high-density regions are formed not only within the elements themselves at the core region, but also by the regions between elements where fibers are interlocked. This latter effect may become excessive ; in certain fiber and element size ranges, and it is desirable in such cases to utilize crimped fibers to control the degree of element interlocking and the compaction.
The packing according to this invention has additional remarkable properties. This packing suppresses wall flow of the :, liquid; that is, flow along the walls of the tower, which occurs with conventional packings. A wiping action has been observed, in the practice of this invention, by the multitude of fibers which engage the tower walls. The liquid which reaches the walls typically from traverse along fibers sloped downwardly towards : .:
the wall, is subsequently picked up by fibers sloped downwardly away from the wall and returned to the packing.
.
`\
105;~85 Anothex featu~e is the internal ent~ainment ellmination pxopexty of this Packing. ~hen the fibexs axe wetted by the liquid, any tendency to strip d~oplets at high gas velocity is compensated by the int~insic droplet-captu~e capability of the adjacent fibers.
Sinoe the point-to-point density of the ~ibexs vaxies, the stripping occu~s in ~egions of low fibex count density and high point gas - velo¢ity. Howevex, the gas must then pass through regions o~ high~iber count density and/or low point gas velooity whexe the entxained d~oplets a~e removed.
Brie~ DescriPtion Of ~he Drawin~s ~or a bette~ understanding of this invention, both as to it~ organization and as to its method of opexation, together with additional objects and advantages thexeof, refexence is made to the following desc~iption, taken in connection with the acoompanying d~awings, in whioh: -~igure 1 is a view in seotion showing a mass-transfex oolumn or towex in accordance with this in~ention;
~ig. 2 is a ~xagmental view enla~ged of a small portion ~;
o~ the bed of the apparatus shown in ~ig. l;
Figs. 3 and 4 axe views in side elevation with the ~ibers '"! omitted fxom the centex showing typical packing bodies ox elements used in the practice of this invention;
~ig. 5 is a fragmental view in side elevation of a fibe~
of the bodies shown in Pigs. 3 and 4;
~ig. 6 is a fxagmental view in side elevation showing the mannex in which a non-wettable fibex oa~ies the liquid in ., the p~actice o~ this invention;
:~ .
~ig. 7 is a ~Yagmental view in side elevation showing ~ the manne~ in which a wettable ~ibex ca~xies the liquid in the - 30 pxactice of this invention; and ~ig. 8 is a g~aph illustxating the opexation of this invention.
, ~ ,:
lOS'~;85 DETAILED DESCRIPTION OF EMBODIMENT
The apparatus shown in Fig. 1 is a column 11 for carrying out a mass-transfer operation typically between a contaminated gas and a liquid to purify the gas. This column 11 includes a shell 13 within which there is a bed 15 for effecting the mass transfer of the contaminant from the gas to the liquid. Near the base of the column there is an inlet 17 for the contaminated gas and near ;
the top of the column 11 there is an outlet 19 for the decontamin- `
ated gas. At the top of the column 11 above the bed 15 there is ;
a spray 21 for distributing the liquid wash over the upper surface of the bed 15. The liquid wash which has absorbed the contaminant may be discarded or returned to the spray 21 through a filter 23 by a pump 25.
The bed 15 is composed of a plurality of cylindrical ~;
bodies or elements 31 randomly disposed within the bed and inter-locked with each other. Each body 31 includes a large number of fibers 33 extending from an axial support 35. The bodies are formed by juxtaposing a pair of wires 37 and 39 parallel to each other, inserting the ends of the fibers 33 to be secured to the axial support between the wires 37 and 39 and twisting the wires into interlaced helices so that they clamp these ends of the -fibers 33. The fibers 33 may be composed of metal, for example, stainless steel, or of plastic, such as polypropylene, polystyrene, "
polyvinylchloride, or fiber glass. The fibers may be crimped as shown in Fig. 5. Figs. 3 and 4 show bodies of typical dimensions.
:: .
: In Fig. 3, x = 3 1/2 inches and in Fig. 4, y = 2 1/2 inches.
A typical body 31 of 3 1/2" diameter and height has 1826 ; fibers 33 extending from an axial support 35 ~aving helices with ; 16 turns. Each fiber has a diameter of .010 inch. The surface ., .
30 area of the fibers on one body 33 is about 200 square inches.
There are about 100 bodies per cubic foot of bed 15 or 140 square feet of fiber contact surface per cubic foot of bed.
:'' '~ .
10~;~685 1 The 2 1/2" diameter body has 909 fibers of .010 diameter each per body. These fibers have a surface area of 71.5 square inches per body. There are about 250 bodies per cubic foot of bed and this provides about 125 square feet of fiber contact area per cubic foot of bed.
The fibers 33 may be non-wettable or wettable by the liquid 41. If the fibers are non-wettable the liquid forms into drops 43 which roll under gravity along the fiber 33a (Fig. 6).
If the fibers are wettable, the liquid flows in a film 45 along 10 the fiber 33b (Fig. 7). ~
The bodies 31 are disposed at random in the bed 15 with -their fibers 33 interlocked. Typically the density of fibers 33 in number or count per unit volume of the fibers at the axis of a body 31 is about twice the density at the periphery. The density of fibers throughout the bed other than at the axes of the bodies 31 depends on the extent to which and the manner in which the fibers 33 are interlocked. The density of fibers from point to point throughout the bed 15 is then highly variable. The spray 41 falling on a region of the bed 15 where the density of fibers is high as near the axis 35 of a body 31 ~Fig. 2) is predominately deflected from this region to other parts of the bed, as shown by ~ the arrows 51 in Fig. 2, and the liquid trickles through the bed - in irregular paths effectively dieontaminating the gas flowing in the opposite direction.
Fig. 8 is a graph showing the relationship between an air mass flow through a bed in accordance with this invention and the pressure drop of the air. The packing elements used are of the type shown in Fig. 4 having a diameter and height of 2 1/2 inches. Air mass flow rate in pounds per hour per square foot of cross section of the tower, disregarding the part of the `~ cross section taken up by the volume of packing, is plotted :
. .
:, .
105'~85 1 horizontally and pressure drop in inches of water per foot of packed depth of the bed is plotted vertically. Both coordinates are logarithmic. Curve A is the plot for dry packing with no wat,er spray; Curve B is the plot for water spray at the rate of 4.38 gallons per minute per square foot; Curve C is the plot for water spray at the rate of 20.7 gallons per minute per square foot. Curve A is linear having a slopeof about 1.8 to 2.0; that is, the pressure drop increases at the rate of about the 1.8 to 2.0 power of the increase in air flow rate. Curve B has a branch Bl parallel to A; the pressure drop for each flow rate for Bl is substantially higher than for A. For example at 2000 lbs/Hr./Ft.2 the pressure drop for A is 0.32 inches of water while for Bl it is 0.45 inches of water. Curve B has another branch B2 which has a higher slope than A or Bl. The break point or loading point between the branches Bl and B2 is at flow rate 2300 lbs/Hr./Ft.2 at a pressure drop of 0.60 inches of water. Curve C likewise has i~ two branches Cl and C2, Cl being parallel to A and Bl but at higher pressure drop at any flow rate. The loading point in this case is at flow rate-2400 - pressure drop 0.68 inches of watqr.
The loading point in each case is the point at which the slope ; of the curve increases above the usuaI 1.8 to 2.0 slope and at which the tendency to flood develops.
Curves B and C show that at any gas-flow rate the pressure drop is higher than for the dry tower. This signifies that the water is being effectively held up by the packing of . . .
fibers 33 in body 31.
The displacement of curves B and C from the dry line A
shows that the water (liquid) is not ~being substantially channeled through the body 31. There would be no substantial displacement 3~ between the curveb if the liquid were channeled. The lower loading points for curve C than for curve B; i.e., lower loading . .
:-~ 05'~point for incxeased liquid flow-rate, also shows the absenoe of substantial channeling.
It has also been found that so e~f0ctive is the packing that if the liquid is impinged as a single stxeam rather than a sp~ay, it is distxibuted throughout the bed within a few packing- -body diameters of downwaxd travel and does not channel.
While pxeiexr0d em~odiments of this invention have been disclosed herein, many modifications thereof are ~easible.
~his invention is not to be restricted except inso~ar as is necessitated by the spixit of the prior axt.
" ~ ,
-This invention relates to mass and/or heat transfer and has particular relationship to mass or heat transfer taking place between counterflowing fluids through packing. ~ass-transfer operations such as gas scrubbing, distillation and the like are carried out by counterflow of a gas and a liquid between which the mass transfer is to take place through a medium whose purpose is to maximize the contact surface or area between the gas and liquid without blocking the gas flow altogether by so-called flooding. Flooding is defined as the limiting. condition which occurs when, as gas or liquid flows are increased, the gas phase becomes discontinuous, the gas-pressure drop becomes unstable, and the bed tends to fill with liquid. Common types of prior-art * *
packing materials include such bodies as Raschig rings and Berl . * Trade Mark . ~
,, -- 1 --j,. '' ,, ~."
,~:
,'.~
~,.,~
.
} .. ~, ~ , . ' ! , ;;~ ~ ' ' ~ '' .
., ,~, ' ~'. ~ '. .' , .
3~
. - . . .
~: ' !
lO~;~S85 1 and Intalox saddles as disclosed in U.S. Leva patent 2,639,909.
These common packings are effective as liquid dispersal surfaces but have the disadvantage of relatively high gas-flow resistance and a susceptibility to flooding at relatively low rates of gas and liquid flow. Design fluid-~low capacities of packed towers are based principall~ on two criteria: the flood limit and the intrinsic gas-flow resistance of the packing. (B.J.Lerner and C.S.Grove, Jr. - Industrial and Engineering Chemistry Vol. 43, pgs. 216-225 Jan. 1951). A consequent disadvantage of such conventional packings in the smaller sizes is the need for un-economically large tower-shell diameter required to keep the gas velocity below the flooding point or to keep gas flow resistance ;
and dependent blower costs within economic limits.
In recent years, commercial packed-tower design practice has been directed toward obtaining higher gas velocities, or low gas flow resistance, and thus more econo~ic smaller tower-shell diameters. Typical of the teachings of the prior-art attempts to ~` meèt this objective are the following U.S.patents:
~ Kleinschmidt 2,143,016 - Smucker 2,607,714 Dixon 2,615,832 - Teller 2,867,425 ~eeping 2,921,776 - Robjohns 3,293,174 Lerner 3,410,057 Lipins~i 3,438,614 ~ These patents disclose beds of randomly disposed packing materials ,` for extending the surface contact between the phases taking part ~`; in the mass transfer. Lower gas-flow resistances and higher gas-; -. .
flow velocities have been achieved through the use of larger sizes of convenkional tower packings such as saddles, and the use of , more "open" distributed-surface packings such as Pall rings and ,., ~ .
~,,, *
Tellerettes (Teller), which flood at much higher liquid and gas ~ flow rates than do the older types of packings. However, in the ... .
,, * Trade Mark : !
r,~
lOS~;85 use of mass tran~fe~ oolumns including paoking o~ this prior-art type there has been experienced the emission o~ liquid spray in large quantities from the top of the ¢olumns, which militates against transfer e~ioiency.
It is an ob~ect of this invention to provide high-oapaoity, high~e~iciency mass~trans~er paoked columns or to~ers whioh sh~ll transmit the gas at relatively high velocities, without exoessive gas-flow resistanoe, shall not ~lood until the liquid and gas-flow rates reach relatively high magnitudes, and ~; 10 shall not em~t spray in large quantities from the top o~ the ; oolumns.
Summa~Y 0~ The Invention It has been discovered from tests o~ the prior-art high-flow-rated beds o~ high-Ilood-point packing structures that theg deYelop a mode o~ ~ailuxe not enco~ntered beiore, ahead o~ the flood point. As gas or li~uid flow is incxeased, beds of these paokings fail first not by ~looding, but by severe spxay or entrainment carxyover. Spray carxyover is the trans~er o~ the liquid in droplets to the gas and the concurrent movement of these droplets by the gas. In most cases, spxay or entrainment oarryover with the gas-ana-liquid system begins in these packings a~ approximately 4 to 6 ~eet per second superfi¢ial gas velocity (based on ~ree tower ¢ross-se¢tional area; i.e., disregarding the volume oc¢upied by the pa¢king) at nom~n~l liquid irrigation rates, and in the absen¢e o~ an ei~icient mist eliminator above the bed, reaches inoperable carryover rates at about 6-8 feet ;~ per second super~ioial gas velo¢ities~
At ga5 velo¢ities greater than 4 to 6 feet per se¢ond for gas densities similar to air at standard atmospheric ¢onditions, liquld tends to be stripped o~ ~n egtended planar sur~a¢e in drop ~ form by gas ~ri¢tion. ~he size o~ liquid drops that can be - supported in an upward-flowing gas stream oan be oalculated b~
. , .
~ 05;~;85 Stokes' law~ but in genexal, the fine~ droplets a~e suppo~ted at the low gas velooities, while la~ge~ and heavie~ drops aYe ent~ained at the highe~ gas velo¢ities. Thus, it has been disoove~ed that in addition to the sp~ay from the top of the ; bed o~ column obseYved with high-velocity ¢onventional paokings, which amountis to a substantial fxa¢tion o~ the liquid input at gas velocities in ex¢ess o~ 5 to 6 feet per se¢ond, thexe is also the isame high degree of baok-sp~ay within the inteYnal voids o~ the packing. ~his inte~nal xeci~oulation of liquid within - 10 a paoked bed employed fo~ oounte~cur~ent gas-liquid oontaoting oausesi depa~tuxe fxom t~ue ¢ounte~ou~ent flow, impai~-s the trans~e~ effi¢iency, and is highly undesixable.
It is an object of this invention to eliminate oY
supp~ess this eife¢t and to p~ovide a packing whiah, by YeaSon oe its gene~al intrinsi¢ st~uotu~e, behaves as an e~i¢ient mist eliminato~, has eiieotive liquid-dispexsal p~ope~ties and yet pYesents to the gas a minimum o~ extended planar su~faoes ~xom . .
which the liquid can be entrained. ;
;. .
~ It has been ~ealized in a~iving at this invention that : -, what is desi~able is packing whose density varies f~om point to point in the bed so as to achieve effective ~adial dispe~sion o~
the liquidO ~he prio~-axt packing does not e~ieotively meet this condition.
Wi~e mesh packings, such as those di~closed by Di~on ;., ~j ~- and Keeping, have uni~o~m capillaYy p~ope~ties, and behave like .,-1 .
:` solid-wall packings when wet. Not only is liquid ~eadily ~e-i~ ent~ained f~om these packings, but these packings are not liquid-dispexsing and they do not se~ve ais e~ficient mist eliminators.
Non-capilla~y fibrous-pellet packings su¢h as those o~ ~exne~
~0 have desirable p~ope~ties; they aYe e~fi¢ient inte~nal mist eliminatoYs. Howeve~, the low and fairly unifoYm spatial density ;' ,:
., ~
~.o5;~85 1 f fibers giving the necessary non-capillarity, yields low liquid retention and causes the liquid at times to channel directly through the packing, so that these packings have low mass-transfer characteristics. Similarly, fiberglass mats, such as those described in Xleinschmidt, suffer from liquid channelling behavior, and are essentially non-dispersive for liquids, giving inferior countercurrent-contact transfer per-formance as compared to planar packings.
In accordance with this invention a new type of packing is provided which has been found to have unique liquid-dispersion properties for effecting gas-liquid contact, and which allows high gas-velocity-low-pressure-drop operation while providing for internal mist elimination. This invention is a mass-transfer or heat-transfer column or tower operating by counter-flow of a gas and liquid having a bed of fibrous bodies or packing elements formed of a multitude of fibers extending radially from a central axial support ~o which the fibers are secured. ~he dimension of the bodies is small relative to the dimension of the column~
Typically the bodies are regularly-shaped, for example of circularly cylindrical form with the height substantially equal to the diameter. The minimum dimension of the column is typically ei~ht to ten times the diameter of a packing~body and the minimum depth of the bed about three times the diameter of the packing ~ body. Typical columns may have a diameter as small as one foot ; and as large as twenty-five feet. The diameter of a packing body should be so related to the density of the radial fibers extending from the axial support that the density of the fibers, in counts per unit volume of the region of fibers, at the periphery of the body is about one-half thedensity or less near the axis of the body.
This invention achieves an important desideration, namely a non-uniform distribution or density of the fibers, in :'~
~0~ 85 I counts per unit volume of the bed from region to region throughout the bed. While this desideration is achieved in a unique and highly advantageous manner with the radial bodies or elements, other modes of achieving this desideration are within the scope of this invention.
In the usual practice of this invention the bodies or elements are randomly disposed in the column with their fibers interlocked. The diameter and/or height of the packing body is large compared to the diameter of the fibers. Typically O the packing body diameter and height are 2 to 4 inches and the diameter of a fiber is .010 to .020 inch. The fibers should be ..
sufficiently strong to resist substantial deformation under the loads impressed on the fibers during mass-transfer operation.
A random bed of fibrous bodies in accordance with this i invention forms an interlocking three-dimensional extended-surface packing with a mar~ed degree of non-uniform spatial density, yielding excellent liquid-dispersion properties, low gas flow resistance, excellent mist elimination characteristics and unique mass-transfer properties. The packing body is very light in .; .
weight and can be made from low-cost, corrosion-resistant ' materials. It is characterized by very high gross void space and very low pressure drops even at high rates of gas and liquid flow. It is highly resistant to both flooding and to internal ~ and external spray carryover.
; A unique feature of the packing in accordance with this ` ~ invention is the variable spatial fiber density of the element, which imparts outstanding advantages over prior-art mesh or fiber . ~
packing elements. The relatively high density of fibers in the axial region around the stem or core of the element causes any , . ~ 30 impinging liquid stream to be intercepted, deflected, dispersed and spread out, generally in the form of multiple smaller li~uid ' ~
105;~685 streams or droplets dixected radial~y away fxom the stem along the ~ibexs. ~his spxeading action ~s independent of the orienta-tion of the element in the bed~ so that the bed is not only highly xesistant to liquid channeling, but achieves a unigue deg~ee o~
xadial dispexsion and re-dispexsion of the liquid.
Depending on the natuxe of the liquid-gas contacting operation, it may be desirable to utilize ~ ~*~si ~hat are either non-wettable or wettable by the liquid phase. ~ox e~ample, in cextain ope~ations, where diffusion xesistanoe within the liquid phase oontxols of~mass txansfex and liquid mixing is desirable ox essential, it is pxefexable to utilize non-wetting fibers so that liquid drops roll along the fibers. ~he rolling o~ the dxops has a stixring action Nhioh enhances the diffusion of the trans-ferxed matter on the surfaoe of the drops throughout the dxops.
Alternately, in certain cases of absorption o~ desorption of a gas ¢omponent to or from the liquid phase (whexe gas diffusion oontxols), it may be desixable to use fibers that are wettable by the liquid, 90 that the liquid is transferxed along the fiber surfaoes as a ¢ontinuous high-sux~a¢e-area thin film. In both ¢ases, non-wettable and wettable fibers, the radial transfer meohanism sexves to transfex liquid fxom the stem xegion to the outer low-iibe~-density xegion of the element whexe the gas pre-domlnately tends to flow be¢ause of the lowe~ flow xesistanoe~
~hus, the unique liquid dispersion me¢hanism sexves to ¢ontinuously txansfeY liquid ~xom regions whexe it would be xelati~ely shielded ~rom buIk-gas-~low ¢ontact to xe~ions whexe the major poxtion of ~; the gas tends te flow. ~uxther, a portion of the fibrous element intexlooks with the peripheral fibexs of its neighboxs, thus allowing the trans~er of liquid from body to body dixe¢tly along ~0 the in~exlocking fibexs. ~iquid that does not txansfex along inte~locking fibers, "dead-ends" at the end of the fiber, and ' .
~05;~685 1 forms drops which then fall through the interstitial space, thus contributing to liquid mixing and redistribution. In the prior-art solid or mesh-surface packings, the free-fall distance of such drops is relatively long, of the order or magnitude of one or more packing diameters, and relatively little mass transfer takes place during this free-fall distance because of the tendency to surface stagnation of small drops. In the fibrous-body bed according to this invention, the free-fall drop distance is a small fraction of the packing diameter because the fibers occupy `
most of the volume of the bed and fiber-to-fiber distances are small. Further, the fibrous packing has a uniquely very large . ~ -number of fiber ends at which free-fall drops are generated.
Gas mixing, which is secured in a prior-art packed bed composed ~-of planar solid bodies by turbulent flow through non-uniform free void volume, is obtained in`the case of the radial fiber-eiement bed according~to this invention by gas flow through volumes , of varying fiber count in the bed or volume density. The high-density regions are formed not only within the elements themselves at the core region, but also by the regions between elements where fibers are interlocked. This latter effect may become excessive ; in certain fiber and element size ranges, and it is desirable in such cases to utilize crimped fibers to control the degree of element interlocking and the compaction.
The packing according to this invention has additional remarkable properties. This packing suppresses wall flow of the :, liquid; that is, flow along the walls of the tower, which occurs with conventional packings. A wiping action has been observed, in the practice of this invention, by the multitude of fibers which engage the tower walls. The liquid which reaches the walls typically from traverse along fibers sloped downwardly towards : .:
the wall, is subsequently picked up by fibers sloped downwardly away from the wall and returned to the packing.
.
`\
105;~85 Anothex featu~e is the internal ent~ainment ellmination pxopexty of this Packing. ~hen the fibexs axe wetted by the liquid, any tendency to strip d~oplets at high gas velocity is compensated by the int~insic droplet-captu~e capability of the adjacent fibers.
Sinoe the point-to-point density of the ~ibexs vaxies, the stripping occu~s in ~egions of low fibex count density and high point gas - velo¢ity. Howevex, the gas must then pass through regions o~ high~iber count density and/or low point gas velooity whexe the entxained d~oplets a~e removed.
Brie~ DescriPtion Of ~he Drawin~s ~or a bette~ understanding of this invention, both as to it~ organization and as to its method of opexation, together with additional objects and advantages thexeof, refexence is made to the following desc~iption, taken in connection with the acoompanying d~awings, in whioh: -~igure 1 is a view in seotion showing a mass-transfex oolumn or towex in accordance with this in~ention;
~ig. 2 is a ~xagmental view enla~ged of a small portion ~;
o~ the bed of the apparatus shown in ~ig. l;
Figs. 3 and 4 axe views in side elevation with the ~ibers '"! omitted fxom the centex showing typical packing bodies ox elements used in the practice of this invention;
~ig. 5 is a fragmental view in side elevation of a fibe~
of the bodies shown in Pigs. 3 and 4;
~ig. 6 is a fxagmental view in side elevation showing the mannex in which a non-wettable fibex oa~ies the liquid in ., the p~actice o~ this invention;
:~ .
~ig. 7 is a ~Yagmental view in side elevation showing ~ the manne~ in which a wettable ~ibex ca~xies the liquid in the - 30 pxactice of this invention; and ~ig. 8 is a g~aph illustxating the opexation of this invention.
, ~ ,:
lOS'~;85 DETAILED DESCRIPTION OF EMBODIMENT
The apparatus shown in Fig. 1 is a column 11 for carrying out a mass-transfer operation typically between a contaminated gas and a liquid to purify the gas. This column 11 includes a shell 13 within which there is a bed 15 for effecting the mass transfer of the contaminant from the gas to the liquid. Near the base of the column there is an inlet 17 for the contaminated gas and near ;
the top of the column 11 there is an outlet 19 for the decontamin- `
ated gas. At the top of the column 11 above the bed 15 there is ;
a spray 21 for distributing the liquid wash over the upper surface of the bed 15. The liquid wash which has absorbed the contaminant may be discarded or returned to the spray 21 through a filter 23 by a pump 25.
The bed 15 is composed of a plurality of cylindrical ~;
bodies or elements 31 randomly disposed within the bed and inter-locked with each other. Each body 31 includes a large number of fibers 33 extending from an axial support 35. The bodies are formed by juxtaposing a pair of wires 37 and 39 parallel to each other, inserting the ends of the fibers 33 to be secured to the axial support between the wires 37 and 39 and twisting the wires into interlaced helices so that they clamp these ends of the -fibers 33. The fibers 33 may be composed of metal, for example, stainless steel, or of plastic, such as polypropylene, polystyrene, "
polyvinylchloride, or fiber glass. The fibers may be crimped as shown in Fig. 5. Figs. 3 and 4 show bodies of typical dimensions.
:: .
: In Fig. 3, x = 3 1/2 inches and in Fig. 4, y = 2 1/2 inches.
A typical body 31 of 3 1/2" diameter and height has 1826 ; fibers 33 extending from an axial support 35 ~aving helices with ; 16 turns. Each fiber has a diameter of .010 inch. The surface ., .
30 area of the fibers on one body 33 is about 200 square inches.
There are about 100 bodies per cubic foot of bed 15 or 140 square feet of fiber contact surface per cubic foot of bed.
:'' '~ .
10~;~685 1 The 2 1/2" diameter body has 909 fibers of .010 diameter each per body. These fibers have a surface area of 71.5 square inches per body. There are about 250 bodies per cubic foot of bed and this provides about 125 square feet of fiber contact area per cubic foot of bed.
The fibers 33 may be non-wettable or wettable by the liquid 41. If the fibers are non-wettable the liquid forms into drops 43 which roll under gravity along the fiber 33a (Fig. 6).
If the fibers are wettable, the liquid flows in a film 45 along 10 the fiber 33b (Fig. 7). ~
The bodies 31 are disposed at random in the bed 15 with -their fibers 33 interlocked. Typically the density of fibers 33 in number or count per unit volume of the fibers at the axis of a body 31 is about twice the density at the periphery. The density of fibers throughout the bed other than at the axes of the bodies 31 depends on the extent to which and the manner in which the fibers 33 are interlocked. The density of fibers from point to point throughout the bed 15 is then highly variable. The spray 41 falling on a region of the bed 15 where the density of fibers is high as near the axis 35 of a body 31 ~Fig. 2) is predominately deflected from this region to other parts of the bed, as shown by ~ the arrows 51 in Fig. 2, and the liquid trickles through the bed - in irregular paths effectively dieontaminating the gas flowing in the opposite direction.
Fig. 8 is a graph showing the relationship between an air mass flow through a bed in accordance with this invention and the pressure drop of the air. The packing elements used are of the type shown in Fig. 4 having a diameter and height of 2 1/2 inches. Air mass flow rate in pounds per hour per square foot of cross section of the tower, disregarding the part of the `~ cross section taken up by the volume of packing, is plotted :
. .
:, .
105'~85 1 horizontally and pressure drop in inches of water per foot of packed depth of the bed is plotted vertically. Both coordinates are logarithmic. Curve A is the plot for dry packing with no wat,er spray; Curve B is the plot for water spray at the rate of 4.38 gallons per minute per square foot; Curve C is the plot for water spray at the rate of 20.7 gallons per minute per square foot. Curve A is linear having a slopeof about 1.8 to 2.0; that is, the pressure drop increases at the rate of about the 1.8 to 2.0 power of the increase in air flow rate. Curve B has a branch Bl parallel to A; the pressure drop for each flow rate for Bl is substantially higher than for A. For example at 2000 lbs/Hr./Ft.2 the pressure drop for A is 0.32 inches of water while for Bl it is 0.45 inches of water. Curve B has another branch B2 which has a higher slope than A or Bl. The break point or loading point between the branches Bl and B2 is at flow rate 2300 lbs/Hr./Ft.2 at a pressure drop of 0.60 inches of water. Curve C likewise has i~ two branches Cl and C2, Cl being parallel to A and Bl but at higher pressure drop at any flow rate. The loading point in this case is at flow rate-2400 - pressure drop 0.68 inches of watqr.
The loading point in each case is the point at which the slope ; of the curve increases above the usuaI 1.8 to 2.0 slope and at which the tendency to flood develops.
Curves B and C show that at any gas-flow rate the pressure drop is higher than for the dry tower. This signifies that the water is being effectively held up by the packing of . . .
fibers 33 in body 31.
The displacement of curves B and C from the dry line A
shows that the water (liquid) is not ~being substantially channeled through the body 31. There would be no substantial displacement 3~ between the curveb if the liquid were channeled. The lower loading points for curve C than for curve B; i.e., lower loading . .
:-~ 05'~point for incxeased liquid flow-rate, also shows the absenoe of substantial channeling.
It has also been found that so e~f0ctive is the packing that if the liquid is impinged as a single stxeam rather than a sp~ay, it is distxibuted throughout the bed within a few packing- -body diameters of downwaxd travel and does not channel.
While pxeiexr0d em~odiments of this invention have been disclosed herein, many modifications thereof are ~easible.
~his invention is not to be restricted except inso~ar as is necessitated by the spixit of the prior axt.
" ~ ,
Claims (8)
1. Apparatus for removing constituents and/or energy from a fluid comprising a packed column having a bed formed throughout of a plurality of fibrous bodies, each of said bodies having an axial support from which fibers extend radially, the said apparatus being characterized by that in said bed of fibrous bodies the bodies are disposed at random with reference to each other with the fibers of contiguous bodies interlocked, so that the number of fibers per unit volume of said bed, varies spatially in all directions from point to point of said bed throughout said bed.
2. The apparatus of claim 1 wherein each body has a volume which is small compared to the volume of the column.
3. The apparatus of claim 1 wherein each body is circularly cylindrical, the number of fibers per unit volume at the periphery of said body being about one-half the number of fibers per unit volume near the axial support of said body.
4. The apparatus of claim 1, for mass and/or heat trans-fer between a liquid and a gas, including means for conducting through the bed a said liquid and a said gas countercurrent to each other.
5. The apparatus of claim 4 for mass and/or heat trans-fer between the liquid and the gas flowing through the bed countercurrent to each other wherein the fibers of each body are wettable by the liquid.
6. The apparatus of claim 4 for mass and/or heat transfer between the liquid and the gas flowing through the bed
6. The apparatus of claim 4 for mass and/or heat transfer between the liquid and the gas flowing through the bed
Claim 6 continued:
countercurrent to each other wherein the fibers of each body are non-wettable by the liquid.
countercurrent to each other wherein the fibers of each body are non-wettable by the liquid.
7. The apparatus of claim 1 wherein the fibers of each of the bodies are crimped.
8. The apparatus of claim 1, for eliminating mist from a mist-laden gas, including means for conducting the mist-laden gas through the bed.
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| US05480702 USB480702I5 (en) | 1974-06-19 | 1974-06-19 |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CA1052685A true CA1052685A (en) | 1979-04-17 |
Family
ID=23909001
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CA223,176A Expired CA1052685A (en) | 1974-06-19 | 1975-03-21 | Removal of mass or energy from a gas in a packed column with fibrous bed |
Country Status (7)
| Country | Link |
|---|---|
| US (1) | USB480702I5 (en) |
| JP (1) | JPS5114175A (en) |
| CA (1) | CA1052685A (en) |
| DE (1) | DE2518484A1 (en) |
| FR (1) | FR2275244A1 (en) |
| GB (1) | GB1500140A (en) |
| IT (1) | IT1039123B (en) |
Families Citing this family (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4203934A (en) | 1975-06-13 | 1980-05-20 | Max Leva | Tower packing element |
| US4229386A (en) * | 1976-08-04 | 1980-10-21 | Lerner Bernard J | Mass or heat transfer or separation of solid or immiscible components from fluids |
| US4277425A (en) | 1978-03-17 | 1981-07-07 | Max Leva | Tower packing element |
| US5261966A (en) * | 1991-01-28 | 1993-11-16 | Kabushiki Kaisha Toshiba | Method of cleaning semiconductor wafers using mixer containing a bundle of gas permeable hollow yarns |
| CN108283850B (en) * | 2017-11-10 | 2020-05-22 | 中国科学院过程工程研究所 | Gas-liquid contact device |
| CN108704429B (en) * | 2018-06-20 | 2021-03-16 | 江苏中科睿赛污染控制工程有限公司 | Industrial rotary atomization washing dust removal device and dust removal method thereof |
| RU2685332C1 (en) * | 2018-12-27 | 2019-04-17 | Общество с ограниченной ответственностью "Компания "СтокамНет" | Fibrous carrier for biomass immobilization |
| CN115335131B (en) | 2020-03-17 | 2024-07-12 | 流体处理有限责任公司 | Coalescing media for hydraulic air and sediment separation device |
-
1974
- 1974-06-19 US US05480702 patent/USB480702I5/en active Pending
-
1975
- 1975-03-21 CA CA223,176A patent/CA1052685A/en not_active Expired
- 1975-03-26 GB GB12736/75A patent/GB1500140A/en not_active Expired
- 1975-04-25 DE DE19752518484 patent/DE2518484A1/en not_active Withdrawn
- 1975-05-14 FR FR7514996A patent/FR2275244A1/en active Granted
- 1975-06-19 JP JP50073825A patent/JPS5114175A/en active Granted
- 1975-06-19 IT IT24546/75A patent/IT1039123B/en active
Also Published As
| Publication number | Publication date |
|---|---|
| DE2518484A1 (en) | 1976-01-08 |
| FR2275244B1 (en) | 1981-12-31 |
| IT1039123B (en) | 1979-12-10 |
| JPS5114175A (en) | 1976-02-04 |
| JPS5429313B2 (en) | 1979-09-21 |
| USB480702I5 (en) | 1976-01-27 |
| FR2275244A1 (en) | 1976-01-16 |
| GB1500140A (en) | 1978-02-08 |
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