Production of pure nitrogen from air

Abstract: A process for removing the impurities carbon monoxide, carbon dioxide, water vapour and, optionally, hydrogen from a feed stream, particularly air, comprises (a) initially removing water and carbon dioxide, (b) catalytically oxidising carbon monoxide and hydrogen to form carbon dioxide and water vapour, respectively, and (c) removing the oxidation products. The resulting gaseous stream may then be separated by cryogenic distillation. A pure nitrogen product can thus be produced. The steps (a) to (c) can be performed by passing the feed gas through a bed comprising at least one first layer of adsorbent for performing step (d), at least one second layer of oxidation catalyst for performing step (b), and at least one third layer of adsorbent for performing step (c). Two or more such beds may be sued with at least one bed being used to product the purified gas while at least one other is being regenerated.

Description: The present invention relates to a process for separating air to produce nitrogen which is free of water vapour, carbon dioxide and carbon monoxide. High purity gases such as nitrogen in which impurities are present in amounts well below part per million levels are required in the manufacture of integrated circuits to prevent defects in chips of increasing line densities. Cryogenic distillation of air is typically used for the production of highly purified nitrogen gas. Removal of impurities from the feed air for cryogenic distillation is required for the production of high purity nitrogen. Impurities, such as H₂O and CO₂, have to be removed to prevent freeze-up in the low temperature sections of the plant. In addition, other impurities, such as H₂ and CO, typically have to be removed from the nitrogen product. A two-step procedure has been employed for the removal of these impurities from air in a nitrogen purification process. In the first step, compressed nitrogen is heated to temperatures between 150° to 250°C and then contacted with a catalyst to oxidise CO to CO₂ and H₂ to H₂O. Noble metal catalysts, typically based on platinum, are commonly used for the oxidation step. In the second step, the oxidation products, CO₂ and H₂O, are removed from the compressed gas stream either by a temperature-swing adsorption process (see K. B. Wilson, A. R. Smith and A. Theobald, IOMA BROADCASTER , Jan-Feb 1984, pp 15-20) or by a pressure-swing adsorption process (see M. Tomonura, S. Nogita, Kagaku Kogaku Ronbunshu , Vol. 13, No. 5, 1987, pp 548-553). These processes, although effective, are disadvantageous for the commercial scale production of highly purified gases, particularly nitrogen gas, as a consequence of their high cost of operation. The cost of operation is high because of the extensive use of noble metal catalysts. In addition, separate vessels must be used for the catalytic treatment step and the adsorption step to remove the impurities. Moreover, heat exchangers are required both to heat the gas as it passes into the catalyst vessel and to cool the effluent therefrom, thereby adding to the cost, both in terms of equipment and energy. Ambient temperature processes for removing parts per million levels of impurities from 'inert gas' streams (e.g. of nitrogen or argon) are also known in the art. Thus U.S.-A-4,579,723 discloses passing an inert gas stream containing nitrogen or argon through a catalytic bed containing a mixture of chromium and platinum on gamma-alumina and a second bed composed of a mixture of several metals mounted on gamma-alumina. The beds effectively convert carbon monoxide to carbon dioxide and hydrogen to water vapour and adsorb the resulting impurities to produce a product stream containing total impurities of less than 1.0 part per million. In addition, U.S.-A-4,713,224 discloses a one-step process for purifying gases containing minute quantities of CO, CO₂, O₂, H₂ and H₂O in which the gas stream is passed through a particulate material comprising nickel having a large surface area. Processes for the ambient temperature conversion of carbon monoxide to carbon dioxide have also for example, been described in U.S.-A-3,672,824 and U.S.-A-3,758,666. None of these processes, however, provides a process in which a gaseous feed air stream which contains up to significant amounts of impurities can be purified by removal of water vapour, carbon dioxide and carbon monoxide to obtain a highly purified air which is subsequently separated to produce high purity nitrogen. According to the invention there is provided a process for separating air comprising (i) purifying a gaseous feed air stream by substantially freeing it of water vapour, carbon monoxide and carbon dioxide impurities by a method comprising the steps of: (a) removing water vapour from the gaseous feed air stream; (b) contacting the feed stream from step (a) with one or more oxidation catalysts thereby to convert carbon monoxide to carbon dioxide; and (c) removing carbon dioxide and, if present, water vapour from the gaseous stream obtained from step (b) to obtain the purified air; and (ii) distilling the purified air to produce nitrogen. If desired, hydrogen impurity may additionally be removed by catalytic reaction with oxygen in step (b) of the process according to the invention. The resulting purified air to be destilled is substantially free of the aforesaid impurities, generally containing no more than about one ppm of carbon dioxide and a combined total of the other impurities not exceeding about one ppm. The gaseous air feed is preferably treated in a single treatment zone, preferably contained in a single vessel which includes a first adsorption section, a catalysis section and a second adsorption section. The first adsorption section contains one or more beds of a water-removing adsorbent, such as activated alumina, silica gel, zeolites or combination thereof. The catalysis section preferably contains (relatively low cost) catalysts for the catalytic conversion of carbon monoxide to carbon dioxide and hydrogen to water vapour. The former catalyst is preferably a mixture of manganese and copper oxides, while the latter catalyst is preferably supported palladium. If the amount of hydrogen in the gaseous air feed is such that its continued presence is not detrimental to the intended use of the purified product, then the catalyst for converting hydrogen to water vapour may be omitted. On the other hand, the production of highly purified nitrogen used in the manufacture of very high density computer chips will require the removal of even the minute amount of hydrogen typically present in air. In accordance with the present invention, such amounts of hydrogen can be removed by converting hydrogen to water vapour using supported palladium or other suitable oxidation catalyst in the catalysis section. The process according to the present invention may be conducted either batchwise or continuously. In either case, the treatment zone containing the two adsorption sections and the catalysis section must be periodically regenerated by purging the accumulated adsorbed impurities. In a batchwise system, purification of the air feed must be stopped during regeneration of the treatment section. In the continuous system, a plurality of treatment zones are used with at least one treatment zone producing purified air while at least one other treatment zone is undergoing regeneration. In accordance with the present invention, the treatment zones may be regenerated by a purge gas at near feed temperatures or at elevated temperatures in a temperature-swing mode. The resulting purified air has no more than about one ppm carbon dioxide and no more than about one ppm total of other impurities. Further particular embodiments of the invention are set out in the dependent claims. The present invention will now be described by way of example with reference to the accompanying drawings in which like reference characters indicate like features and in which: FIGURE 1 is a schematic view of one apparatus for performing steps (a) to (c) according to the invention showing a continuous process for the production of highly purified air utilising a pressure-swing mode of operation; FIGURE 2 is a schematic view of another apparatus for performing steps (a) to (c) according to the invention, in which a temperature-swing mode of operation is utilised; and FIGURE 3 is a schematic view of an apparatus for performing the method according to the invention including the apparatus shown in Figure 2 in combination with apparatus for separating the resulting purified air in a cryogenic distillation system. The process according to the present invention typically produces highly purified nitrogen with regard to the impurities carbon monoxide, carbon dioxide, and water vapour. It is to be understood that the term "impurities", as used herein, refers to these gases and does not include other gases such as, for example, trace amounts of hydrocarbons, which might be present in a feed air mixture and which may otherwise be regarded as impurities. It is further to be understood that the feed air mixture contains at least carbon monoxide. Carbon dioxide and water vapour are also present in the initial feed stream and may be generated during the oxidation step of the process. Referring to the drawings, and particularly to FIG. 1, there is shown an apparatus for operating a continuous process for the production of purified air in which a treatment zone undergoing regeneration is purged with a gas at or near the temperature of the air feed. A feed air stream, as for example atmospheric air, is passed via a line 2 to a compressor 4 wherein the air is compressed to about 0.62 to 1.13 MPa (75 to 150 psig). The compressed air stream then passes via a line 6 to a heat exchanger 8 wherein it is cooled upstream of its introduction via line 10 into a water separator 12 to remove liquid water therefrom. The effluent from the water separator 12 is at a temperature of from about 5°C to 50°C, preferably from about 20°C to 45°C. The air stream then flows via a line 14, a valve 16 and a line 20 to a treatment zone 29 within a single vessel 30 which contains a lower adsorption section 34, a catalysis section 38, and an upper adsorption section 42. The lower adsorption section 34 contains at least one bed (or layer) of a water removing adsorbent material such as activated alumina, silica gel, zeolites or combinations thereof which removes water vapour and some of the carbon dioxide present in the compressed air stream. Most of the water vapour remaining in the compressed air is removed in the lower adsorbent section 34 in order to prevent deactivation of the oxidation catalysts present in the catalysis section 38 and to permit low temperature processing of the feed. Preferably, the adsorption section 34 comprises a predominant layer of activated alumina or silica gel and a layer of zeolite, for example, Zeolite 13X or 5A manufactured by UOP, Inc. The air stream then enters the catalysis section 38 within the treatment vessel 30. The physical separation of the three sections of the treatment vessel 30 is effected by means well known in the art. For example, the adsorption section 34 and the catalysis section 38 may be separated by a stainless steel screen. A similar screen may also be employed to separate the catalysis section 38 from the upper adsorption section 42. The catalysis section 38 contains a catalyst for the oxidation of carbon monoxide to carbon dioxide and a catalyst for the conversion of hydrogen to water vapour. The catalyst used for eliminating carbon monoxide is preferably a metal oxide such as nickel oxide or a mixture of oxides of manganese and copper. The catalyst used in the oxidation of hydrogen to water vapour is preferably supported palladium or another noble metal catalyst known in the art. Preferably, the air stream contacts the carbon monoxide oxidation catalyst upstream of the hydrogen oxidation catalyst. The thus-treated air enters the upper adsorption section 42 for removal of carbon dioxide and water vapour. The adsorbent that may be used in the upper adsorption section 42 preferably includes a zeolite, activated alumina, silica gel and combinations thereof. The thus treated purified air typically containing no more than about 1.0 ppm carbon dioxide and no more than about one ppm of the total of other impurities is withdrawn from the treatment vessel 30 and flows through a line 46 and a valve 58 to a line 62 where it is sent to storage or for further processing such as by cryogenic distillation. At the same time the treatment zone 29 is purifying the air feed, a treatment zone 31 is undergoing regeneration to remove accumulated impurities. The treatment vessel 32 is essentially the same as treatment vessel 30 and contains a corresponding lower adsorption section 36, a catalysis section 40 and an upper section 44. The structure of the three sections 36, 40, 44 and the materials contained therein are the same as described above for the sections 34, 38, 42, respectively. After purifying the feed air for a period of time, each of the lower and upper adsorption sections 36 and 44 becomes contaminated with carbon dioxide and water, and the catalysis section 40 accumulates small amounts of carbon monoxide and hydrogen. These impurities are removed by purging the vessel 32 with a gas which does not adversely affect the catalyst and is free of the impurities that are to be removed from the vessel 32. For example, as the feed gas is air, a suitable purge gas can be highly purified nitrogen, oxygen or mixtures thereof. Prior to introduction of the purge gas, the vessel 32 is vented to reduce the pressure therein to close to atmospheric. This is carried out by opening valve 26, thereby venting gas through a line 22 and an exit line 28. Referring further to FIG. 1, a purge gas obtained from an independent source (not shown) as a side stream from a line 62 (communicating with the line 46), or as a waste gas from a cryogenic distillation column (not shown) at a pressure of from about 107 - 135 kPa (1-5 psig) is fed via a line 70 to an optional blower 68 where the pressure may be raised, if necessary. The gas flows via the line 66 to a line 54 and through a valve 52 into a line 48 where the purge gas enters the vessel 32. The purge gas exits the vessel 32 through a line 22 and flows through a valve 26 and is thereafter discharged via a line 28. During this operation, the valve 24 connected to the line 20 is closed. After purging, it is preferred gradually to build up the pressure in the vessel 32 with purified air, referred to as "product backfill" in TABLE I. This repressurising may be accomplished by diverting a small portion of the purified air from the line 46 through a valve 56 and into the vessel 32 via the line 48. Once purging and repressurisation are completed, the vessel 32 is again ready to begin a purification cycle. This is done by closing the valve 16 and opening the valve 18 so that the air stream flows from the line 14 to the line 22 and into the lower adsorption section 36 of the vessel 32. The purified air obtained from the vessel 32 passes through the line 48 and a valve 60 into the exit line 62. At the same time, closing of the valve 16 the flow of the air feed stream to the vessel 30 to be terminated. Regeneration is commenced by first venting the vessel 30 and then introducing purge gas via lines 66, 54, and valve 50 into the line 46. The time for completing a cycle in the pressure-swing mode of operation is typically from about 6 to 40 minutes. The cycle for the two-vessel process described in FIG. 1 is shown in TABLE I. Step Typical Valves Open Time(sec) a. Purify using vessel 30, vent vessel 32 to atmosphere 16,26,58 30 b. Purify using vessel 30, regenerate vessel 32 with impurity-free gas 16,26,52,58 510 c. Purify using vessel 30, backfill vessel 32 with vessel 30 product 16,56,58 60 d. Purify using vessel 32, vent vessel 30 to atmosphere 18,24,60 30 e. Purify using vessel 32, regenerate vessel 30 with impurity-free gas 18,24,50.60 510 f. Purify using vessel 32, backfill vessel 30 with vessel 32 product 18,56,60 60 Total Time: 20 minutes. The process according to the present invention can also be carried out by heating the purge gas to temperatures well above the temperature of the feed stream. In this temperature-swing mode of the operation, the temperature of the feed air is cooled to generally below the temperature of the feed air employed in the pressure-swing embodiment, preferably in the range of from about 5° to 20°C. Referring to FIG. 2, the temperature-swing mode of operation commences by pressurising the feed air stream in the compressor 4 to a pressure of from about 0.62 to 1.13 MPa (75 to 150 psig). The compressed air stream is then passed to a heat exchanger 8 through the line 6 and then to the water separator 12 through the line 10. The compressed air exiting the water separator 12 is preferably at a temperature of from about 5° to 20°C. The operation of the purification treatment zones 29 and 31 is the same as that described in connection with the apparatus shown in FIG. 1. In the temperature-swing mode of operation shown in FIG. 2, the vessels 30 or 32 are normally pressurised slowly using feed air and the product backfill step as described with reference to that in the pressure-swing mode of operation. For the repressurisation of vessel 30, the valve 16 will be open while valve 18 is utilised for the repressurisation of the vessel 32. After the repressurisation of the vessel 30, purification of the feed air takes place and the highly purified product air is sent via the line 62 for downstream processing in a cryogenic distillation system. During purification in the vessel 30, the vessel 32 is first vented through the valve 24 and the line 28 and then regenerated using impurity-free purge gas which is passed to an optional blower 68 and then to a heater 64 via the line 66. The temperature of the purge gas entering the system through line 70 is generally close to that of the feed air. Therefore, the purge gas is heated in the heater 64, preferably to a temperature of from about 80° to 250° C. The heated regeneration gas passes through the line 54, the open valve 52 and the line 48 to vessel 32 and then to the line 28 via the open valve 26, thereby removing previously adsorbed impurities. The heat supplied to the vessel 32 by the purge gas is sufficient to desorb the impurities contained therein. Accordingly, it is preferable to turn off the heater 64 after sufficient heat has been introduced into the vessel 32. The amount of heat required for a given vessel can be routinely determined. The flow of purge gas continues after heater 64 has been turned off to remove desorbed impurities and to begin to cool the vessel 32 in preparation for the next purification step. After the vessel 32 is cooled sufficiently, it is slowly repressurised using a portion of the feed air through the open valve 18 and the line 22. The vessel 30 continues to purify the feed air during this time. After repressurisation of the vessel 32, the vessel 30 undergoes the steps of venting, heating with purge gas and cooling with purge gas as described for the vessel 32. Simultaneously, the vessel 32 is purifying feed air. The process can run continuously in this manner. The complete cycle time for the temperature-swing process described in FIG. 2 normally is from about 8 to 24 hours, much longer than the cycle times for the pressure-swing mode of operation. A complete cycle for a two-bed process operated in the temperature-swing mode is given in TABLE II below. Step Typical Valves Open Time (hours) a. Pressurise vessel 30 with feed, purify using vessel 32 16,18,60 0.25 b. Purify using vessel 30, vent vessel 32 to atmosphere 16,26,58 0.25 c. Purify using vessel 30, regenerates vessel 32 with hot purge gas 16,26,52,58 2.5 d. Purify using vessel 30, cool vessel 32 with purge gas 16,26,52,58 5.0 e. Purify using vessel 30, pressurise vessel 32 with feed 16,18,58 0.25 f. Purify using vessel 32, vent vessel 30 to atmosphere 18,24,60 0.25 g. Purify using vessel 32, regenerate vessel 30 with hot purge gas 18,24,50,60 2.5 h. Purify using vessel 32, cool vessel 30 with purge gas 18,24,50,60 5.0 As previously described in connection with FIG. 1, the purge gas should be free of the impurities to be removed by the system (i.e. substantially free of carbon monoxide, carbon dioxide, hydrogen and water vapour) and should not adversely affect the components of the three sections of the vessel. If the purified air exiting the line 62 is sent to a cryogenic distillation system for further processing, the waste gas exiting the cryogenic system may be advantageously used as the purge gas. A system for transferring the purified air to a cryogenic distillation system is shown in FIG. 3. The purified air stream exiting at line 62 is cooled in a heat exchanger 76 against returning product streams 78 and 86 and purge gas stream 80. The warmed product streams 72 and 74 are taken as products and sent to user equipment or storage. The warm purge gas stream 70 is used to regenerate the purification vessels as mentioned earlier. The cold purified air stream 82 exiting the exchanger 76 is further cooled in a turboexpander 84 to produce a stream 88 which is distilled at cryogenic temperatures in a column 90 to produce two product streams 86 and 78 and a waste stream 80 which is used as the purge gas. The cryogenic distillation system is typically of a conventional kind whose operation and construction is well known in the gas separation art. The process according to the invention is further illustrated by the following examples. EXAMPLE I A single-vessel process was operated in a pressure-swing mode. The vessel contained an initial layer of 12.26 kg (27 lbs.) of a commercially available activated alumina, then a layer of 0.77 kg (1.7 lbs.) of 6x14 mesh Hopcalite (a mixture of manganese and copper oxides manufactured by MSA of Pittsburgh, Pennsylvania) and a final layer of 5.27 kg (11.6 lbs.) of the activated alumina. Water-saturated feed air at a temperature of 25°C, a pressure of 1.07 MPa (140 psig), a flow rate of 0,65 m³/min (23.0 std. cubic feet per min.), and containing about 350 ppm CO₂ was passed through the vessel using the cycle sequence shown in TABLE I. Carbon monoxide at a controlled flow rate was blended in the feed air to give a feed gas stream carbon monoxide concentration of 5.5 ppm. The vessel was regenerated at the feed temperature (25°C) using impurity-free nitrogen at an average flow rate (averaged over the entire cycle) of 16,6 m³/min (9.7 std. cubic feet per sec). The gas exiting the vessel contained less than 0.1 ppm H₂O, 1 ppm carbon dioxide and no carbon monoxide. The carbon monoxide in the feed air was converted to carbon dioxide by the Hopcalite layer and the remaining carbon dioxide and the oxidation producers were removed by the second activated alumina layer. EXAMPLE II A single vessel similar to that in Example I was loaded with a first layer of 12.26 kg (27 lbs.) of commercially available activated alumina, a second layer of 0.77 kg (1.7 lbs.) of 6x14 mesh Hopcalite, a third layer of 0.68 kg (1.5 lbs.) of a catalyst containing 0.5% by weight palladium supported on alumina (manufactured by Engelhard Corporation) and a final layer of 4.54 kg (10 lbs.) of activated alumina. The process was operated under the same conditions of Example I with the feed air containing 5.5 ppm of added CO and 2.0 ppm of added hydrogen in addition to the amounts of H₂O and CO₂ stated in Example 1. The gas exiting the vessel contained no H₂ no CO, less than 0.1 ppm of H₂O and less than 1 ppm of carbon dioxide. EXAMPLES III-VI The process of the present invention was conducted in accordance with the scheme shown and described in FIG. 2 wherein the purge gas was heated to a temperature exceeding the temperature of the feed gas air. The lower adsorption section 34 of the vessel 30 was charged with a layer of 5.23 kg (11.5 lbs.) of activated alumina having thereon a layer of Zeolite 13X in an amount of 2.59 kg (5.7 lbs.). The catalysis section 38 was charged with 0.32 mm (1/8") Carulite 200 pellets (a mixture of manganese and copper oxides manufactured by Carus Chemical Company of Ottawa, Illinois) in the amounts shown in TABLE IV. The upper adsorption section 42 was provided with 2.45 kg (5.4 lbs.) of Zeolite 13X. A water-saturated air stream pressurised to 0.65 MPa (80 psig) containing about 350 ppm of carbon dioxide and varying amounts of carbon monoxide was forwarded to the vessel 30 at the rate of 0.82 m³/min (28.8 standard cubic feet per min.). Simultaneously, a regeneration flow of a purge gas at the rate of 0.14 m³/min (5.1 standard cubic feet per min.) was used to remove impurities from the vessel 32. At a feed temperature of 4.4°C, a regeneration gas temperature of 121°C, was used. Using a higher feed temperature of 12.5°C, a regeneration gas temperature of 148.9°C was used. The time necessary to perform each step of the purification and regeneration cycles is shown in TABLE III. Step Time (hr.) Vessel pressurisation 0.2 Feed purification 6.0 Vessel venting 0.1 Heating with impurity-free nitrogen 3.5 Cooling with impurity-free nitrogen 2.2 Total 12.0 hrs. As seen from TABLE III, the time used to complete a single cycle of purification and regeneration is 12.0 hrs. during the temperature-swing adsorption mode or approximately twenty times longer than the time needed to complete a single cycle in the pressure-swing adsorption mode of operation. TABLE IV shows that in each of EXAMPLES III-VI, the conversion of carbon monoxide to carbon dioxide is very high. This is accomplished at very low feed temperatures in accordance with the present invention in part because substantially all of the water vapour has been removed. Example Number Feed Temp. (°C) ((°F)) Feed CO Conc. (ppm) Amount of Carulite (kg) ((lbs.)) Av. Conversion of CO to CO₂ (%) III 4.4 (40.0) 9.0 1.36 (3.0) 92.0 IV 4.4 (40.0) 4.9 1.36 (3.0) 95.0 V 12.5 (54.5) 4.9 1.36 (3.0) 100.0 VI 4.4 (40.0) 4.9 2.0 (4.5) 100.0 In all examples, the gas exiting the lower adsorption section contained less than 0.1 ppm of water vapour and the gas recovered from the upper adsorption section contained less than 1 ppm carbon dioxide.

Claims: A process for separating air comprising (i) purifying a gaseous feed air stream by substantially freeing it of water vapour, carbon monoxide and carbon dioxide impurities by a method comprising the steps of: (a) removing water vapour from the gaseous feed air stream; (b) contacting the feed stream from step (a) with one or more oxidation catalysts thereby to convert carbon monoxide to carbon dioxide; and (c) removing carbon dioxide and, if present, water vapour from the gaseous stream obtained from step (b) to obtain the purified air; and (ii) distilling the purified air to produce nitrogen. A process according to Claim 1, wherein step (a) comprises contacting the gaseous feed stream with a water vapour-removing adsorbent. A process according to Claim 2, wherein the water vapour-removing adsorbent is selected from the group consisting of activated alumina, silica gel, zeolites and combinations thereof. A process according to any one of the preceding claims, wherein the oxidation catalyst in step (b) is a mixture of manganese and copper oxides. A process according to any one of the preceding claims, in which the said gaseous feed air stream is also substantially freed of hydrogen, wherein in step (b) the feed from step (a) is additionally contacted with an oxidation catalyst to convert hydrogen to water vapour. A process according to claim 5, wherein the oxidation catalyst for converting hydrogen to water vapour is supported palladium. A process according to any one of the preceding claims, wherein the feed stream is compressed to a pressure in the range of from 618 to 1135 kPa (75 to 150 psig) upstream of step (a). A process as claimed in any one of the preceding claims, in which the said steps (a) to (c) are performed by passing the feed gas through a bed comprising at least one first layer of adsorbent for performing step (a), at least one second layer of oxidation catalyst for performing step (b), and at least one third layer of adsorbent for performing step (c). A process according to claim 8, wherein a plurality of said beds are used, at least one of said beds being used to remove said impurities from said gaseous feed stream, and at least one of said beds being simultaneously purged to remove said impurities contained therein. A process according to claim 8, wherein the step of purging comprises reducing the pressure in the bed, and passing a purge gas therethrough at a pressure below the pressure of the feed stream and at ambient temperature, said purge gas being substantially free of said impurities. A process according to claim 8, wherein the step of purging comprises reducing the pressure in the bed and passing a suitable purge gas therethrough at a temperature in the range of from 80° to 250°C, said purge gas being substantially free of said impurities. A process according to claim 11, further comprising passing an additional amount of purge gas through the treatment zone to reduce the temperature thereof. A process as claimed in any one of the preceding claims, in which in step (a) carbon dioxide impurity is also removed from the feed stream by adsorption. A process as claimed in claim 13, in which in both steps (a) and (c) there is employed a first adsorbent for removing water vapour and a second adsorbent for removing carbon dioxide.

Inventors: JAIN RAVI, JAIN, RAVI
Applicants: BOC GROUP INC, THE BOC GROUP, INC.
Application year: 1991
Main classification: B01D53
IPC codes: B01D53, F25J3, C01B21, B01J23