JPS598602A - Method of separating hydrogen from mixed gas - Google Patents

Abstract

(57) [Summary] This bulletin contains application data before electronic filing, so abstract data is not recorded.

Description

DETAILED DESCRIPTION OF THE INVENTION The present invention relates to a method of separating hydrogen from a mixed gas stream using hydrogen.

Two methods are commonly used to purify and separate hydrogen-containing mixed gas streams. In the first purification method, the contaminants are adsorbed and the 'nI hydrogen passes through the layer; in the other, the hydrogen is removed by contact with a hydrogenatable material and the contaminants pass through the layer. passing through. The patents relating to the first method (II page 5) are listed below; U.S. Pat. A multi-stage reactor adiabatic pressure swing cycle is disclosed for purifying hydrogen-rich (97+) gas streams by absorbing and passing hydrogen through in pure form.

The above US patent further describes suitable combinations of adsorbents selected with respect to their combined heat capacity, thermal conductivity and density, such as 6-10 US standard mesh silica gel and granular (6-10 US standard mesh) aluminum. or in combination with other materials such as iron or steel, suggesting adjustment of temperature fluctuations within the bed between adsorption and desorption cycles to reach isothermal operation.

U.S. Pat. No. 3,141,748 discloses a method for recovering pure hydrogen from a vapor stream containing hydrogen and a mixture of hydrocarbon compounds. In this method, an adsorbent with a greater affinity for hydrocarbons than for hydrogen, such as activated carbon or alumina, is selected (page 6), and the hydrogen is relatively pure (99,000 mol. - cent hydrogen) as a flow through the absorbing layer. A two-step depressurization step method is used.

A second type of hydrogen purification process uses hydridable materials, where such materials are chemically combined with hydrogen to form metal hydrides. Therefore, hydrogen is adsorbed and pollutants pass through, unlike the methods described above. The following patents relate to hydrogen separation or storage and storage methods using hydrogenatable materials; U.S. Pat. No. 3,793,435 deals with hydrogen
Na r CO + co2. A method for separating H8o and CH from other gaseous substances is disclosed. Separation is carried out by contacting the gas mixture with an alloy of rare earth lanthanum in a distributed configuration and nickel in an active state, the metals forming hydrides upon contact with hydrogen. The mixed gas is passed through a tubular reactor containing an inert highly porous packing material at an initial pressure of 175 psia to prevent agglomeration at room temperature, the effluent gas is removed at a pressure of 116-133 psia, and then the pressure to 25 psia (7th
Page) Hydrogen is separated by desorption.

U.S. Pat. No. 4,036,944 discloses an isothermal method for recovering hydrogen from mixed gas and waste gas streams, particularly refinery Kang et al. waste gas streams, using hydrogen solvents.

The hydrogen absorbent includes a hydrogenatable material, such as an alloy of 5 nickel lanthanum, and a polymeric binder. The absorbent optionally contains inert ingredients such as copper, nickel or iron. Such components are said to be useful for cooling heat sinks and thermal modifiers in adsorption processes. Certain polymeric binders improve the abrasion resistance of IJ Lux hydrogen absorbers; such binders include block copolymers of polystyrene-polybutadiene and polyisolune-polystyrene. Examples include reactor tubes filled with absorbent-binder pellets and a jacket around the reactor for passage of cooling water to maintain isothermal conditions. The use of a fixed bed reactor is shown.

Pellets of lanthanum nickel powder containing 15 g of water glass and lanthanum nickel-copper powder mixture without polymeric binder (addition of copper powder up to % by weight) are used to reduce expansion. There is. The resulting product expanded by more than 4 cm during hydrogenation and collapsed after two cycles of hydrogenation.

U.S. Pat. No. 4,185,979 discloses a method for transferring heat to and from a metal hydride contained in a storage vessel. In the prior art, tubes are placed at regular intervals throughout the bed of hydride material, and a heat exchange material is circulated outside these tubes to heat and cool the reactor as desired.

Other methods have used the gas itself as a means to form or cool the gas stream for absorption or desorption as desired.

US 14F No. 4,108,605 discloses a method for treating a mixture of hydrogen and impure gases by passing the gas through a hydride vessel in which absorption of the hydrogen takes place by a hydride-forming substance. To facilitate the absorption and release of hydrogen and impurities from the 7yC compound-forming material,
Cooling Fluid Bo/Zo, Heat Exchanger and Heating (Page 9) A fluid pump and a heat exchanger are provided.

U.S. Patent Nos. 4,079,523 and 4,096,63
No. 9, No. 4.096,641 and No. 4,079,52
No. 3 discloses various hydrogenatable alloys suitable for recovering hydrogen from gas streams.

U.S. Patent Nos. 4,135,621 and 4,134,49
No. 0, No. 4,134,491 and No. 4,133,42
No. 6 discloses the use of solid elongated particles of low apparent density distributed within the confines of a metal hydride as a system for storing hydrogen. hydrogenatable metals and granular solids,
That is, a mixture with metal powder, such as nickel powder, is added to the hydrogen storage container. Also disclosed is the use of dry diatomaceous earth, lignin, and metal whiskers combined such that the packing density is no greater than 8 degrees of theory of the powder itself. The Taa patent discloses the use of collapsible structures.

In another paper, Sandozuk et al.
tal) discloses an adiabatic method that uses a thermal ballast with a hydride storage material to recover the energy generated during exothermic hydrogenation, and the recovered energy is stored within the thermal ballast (page flilo). be done. Examples are:
The use of a bath of water or molten sodium sulfate, decahydride as a thermal pallad in the reservoir to recover the heat generated during hydrogenation, and the recovery of heat from the reservoir bath to enhance desorption.

The present invention relates to an improved adiabatic method for separating hydrogen from a gas mixture. The improvements of the present invention allow fast cycle times to be achieved using minimal energy requirements and superior bed efficiencies. The improvements to the adiabatic hydrogen separation process consist of: (a) The composite is controlled by the initial hydrogen pressure, hydrogen concentration and temperature (
Moving from Pz r ”x , Tz ) to the final hydrogen pressure, hydrogen concentration and temperature (P21 CII, Ta), P, I
is larger than P□, CII is C1, and Sho is also Ohata, so C4-
C1 dominates the theoretical hydrogenation capacity by at least 5o, Tl
comprising a homogeneous composite of a material capable of hydridation and an inert thermal ballast under conditions where l is greater than T↓, such that the composite absorbs at least 50 g of the theoretical energy of the hydride material; (p. 11) passing a hydrogen-containing gas mixture through the skin containing the above amount of buffst (page 11); (b) reducing the pressure and utilizing the hydride formation energy for desorption; to desorb hydrogen from the layer.

By carrying out the method of the invention in the manner described above, the heat of reaction retained within the composite is utilized to achieve an adiabatic pressure swing process for hydride desorption, resulting in very fast absorption and desorption. You can get speed. Furthermore, the layer can be used considerably, e.g. 50% or more, minimizing wear of the hydridable material since the thermal parast is in intimate contact with the hydridable material, and reducing the distance between the system and the external environment. energy transfer can be kept to a minimum.

The present invention will be described in detail below with reference to the accompanying drawings.

To facilitate an understanding of the significance of the present invention, particularly the use of external thermal ballasts or composite materials of hydridable materials and thermal ballasts for isothermal operations, reference is made to FIG. Figure 1 shows two isothermal equilibrium curves for the LaN13Ha system at ℃ and 100℃, where the logarithm (vertical @) of the hydrogen partial pressure (p) is the layer volume It i.e. hydrogen to metal ratio (H/
M) is illustrated.

For example, referring to diagram #I1, the starting point for the method of the present invention is that the hydrogen partial pressure (P) is 50 psi and the initial hydrogen concentration is 0.
At a starting condition of 1.38'C (Tl), 38"C
Point A is a point along the isothermal curve. When pressurizing an adiabatic reactor containing a non-ballasted hydride-forming metal material, the partial pressure P, along the line A-B' across the pressure and filling curve, is Hydrogen concentration C1
A point B' with / is reached. In this system, C, I and 0
As can be seen from the difference between 0 and 0, only a small amount of hydrogen is absorbed. In a partially ballasted system, the hydridable metal material crosses line A-B. Therefore, the terminal equilibrium state obtained by the reaction mass is achieved at a point at the higher loading end of the 100'C isotherm, ie at point B. However, the amount of ballast can be adjusted as shown below so that a substantially complete filling corresponding to B" on the 100° C. isotopic curve can be achieved. In an isothermal system, the path (Page 13) Continue on the isotherm to point C.

The conventional problem is that absorption and desorption along path A-B'', in an adiabatic system along path A-H, and in an isothermal system along path A-C is particularly large in the reactor. This has limited the commercial use of hydrogenatable materials in performing the separation of gas mixtures.In the present invention, the use of hydrogenatable materials in a spatially distributed configuration for adiabatic methods has been limited. By using a composite material of a hydridable material and a thermal pallast having a specific relationship, the line A-B", and more generally the path A -Tracing B is an OT ability.

Ballast materials, in which hydridable materials are bound together in a spatially distributed manner to form composite materials, are inert, small particulate materials such as steel, nickel, aluminum or iron. Normally, the ballast has good thermal conductivity and a particle size of about 1-100f of the particle size of the hydrogenatable material after hydrogenation (but not exceeding 4 meshes, (It is convenient if it is less than Messier)
. In many (#114) cases, the particle size diameter of the hydrogenatable material after hydrogenation is sub-diameter to 100 mesh and the p1 ballast is of similar size.

The term "spatially distributed" used to describe a pallast material indicates a pallast material that is randomly distributed and exists as individual particles in contact with the hydridable material. Additionally, the pallast material is sintered with a hydridable material to
Palast material present as a network structure, such as obtained by forming an integral composite structure bonded to the ballast, in particular 5androck' at al.
Ballast material in the form of pellets disclosed in the U.S. Patent Application filed in the name of U.S. Pat. or ballast material present as multispecies pellets: any combination of the above, e.g. a network structure with randomly distributed particles, or randomly distributed equiaxed particles with randomly distributed particles. Used to refer to pallast material present as pellets in combination with distributed fine wire-like or fiber-like particles (page 15).

In adiabatic reactors, the amount of thermal sieving used in the composite partially controls the amount of hydrogen removed from the feed stream. Other factors include the hydrogen partial pressure of the feed stream. ,
These include the type of hydrogenatable material, the temperature and rate of the feed stream, the desired hydrogen recovery pressure, etc. If the amount of thermal ballast is too small, the entire reactor mass (thermal ballast plus hydridable material) will be heated by the exothermic hydrogenation reaction at temperature Tat, so that the hydridable material will be completely converted to hydride. The hydrogenation reaction stops earlier. Temperature T11 is determined by the hydrogen partial pressure within the feed stream and the pressure-temperature relationship that exists for the particular hydrogenatable substance. If the thermal ballast exceeds a critical amount, the energy provided by the exothermic hydrogenation reaction will be insufficient to heat the reactor to T2. In this case, the hydrogenation reaction proceeds rapidly to completion, but the final temperature of the reaction mass is lower than the desired value Ta. This low temperature indicates that the bed volume is not used effectively and that the hydrogen pressure obtained during desorption is low.

If the desired amount of thermal ballast is used, the reaction mass will rise from the starting temperature T1 to the final temperature Tg just when the hydrogenatable material is completely hydrogenated, and the weight of such electrically conductive thermal ballast will increase. The ratio of hydridable material to stoichiometric ratio is called the stoichiometric ratio.

In the present invention, at least 50% of the theoretical ratio, preferably 90q6, without the use of external ballast or heat transfer means.
It is necessary to provide sufficient thermal ballast to achieve this. It is undesirable to use excess ballast. Therefore, a ballast with a theoretical ratio (a) in the range of -150 yen is used.

The minimum required amount of ballast material to achieve the above levels is determined by ascertaining the initial temperature, calculating the heat absorption characteristics of the hydridable material and the ballast, and determining the amount of hydridable material present. Check the heat released by hydrogenation (△H), check the temperature at which the equilibrium pressure of hydrogen on the hydride is equal to the partial pressure of hydrogen in the feed gas, check the initial temperature (Tl) and the maximum punch temperature (page 17). ) Measure △T by the difference from (T2), and calculate the unknown amount of ballast from the relationship between △T and the total heat absorption amount △H of the materials present in the reactor as shown in the formula below. determined by. ΔT is at least 10°C and generally within the range of +80°C.

It is advantageous to use pellets containing pallast material as pellet binder rather than using polymeric binders. Such pellets transfer heat much more easily and have faster absorption and desorption rates. In this respect, L
It is convenient to form pellets by sintering a hydridable material such as aNi5 and nickel or other sinterable metal powder. Sintering is conveniently carried out by heating a mixed amount of LaNi5 and metal powder which have been formed into pellets by pressure or other methods (eg extrusion and slicing). In the case of nickel, sintering can be carried out at temperatures of about 700°C to about 900°C for about 0.1 to about 2 hours.

The hydride-forming material and ballast powder were combined at approximately O1 to O5.
Pellets can also be formed by combining with a resin binder such as a silicone rubber in a heavy tS proportion. This solid mixture typically has a tli of about 4 grams and is in the form of a cylinder 1.5 inches tall and IA inch diameter.

It is advantageous to use a high pressure pelletizer capable of producing pellets under pressures of 1.000 to 30,000 psl. Prior to use, the pressurized pellets can be cut into segments, eg, quarter-cylindrical, about 1/4 inch on a side. The purpose of cutting the ilenotated composite is to increase the surface area of the entire composite for hydrogen reaction and desorption. The cut pellets are advantageously further activated prior to use, for example by exposure to high pressure hydrogen. However, as can be seen from the examples, the plastic or island binder inhibits heat transfer within the pellet, often leading to inappropriate reaction front lengths and front velocities.

(Page 19) What is important about the workability of the present invention, especially the rapid adsorption and release of hydrogen by a material that can be hydrogenated in a short cycle time of, for example, 10 seconds or less, is the thermal ballast and hydrogenation process. The goal is to speed up the removal or supply of heat to the reactant particles by shortening the heat transfer path for the amount of material available. The heat transfer path can be ensured by mixing small particles of thermal ballast material and hydrogenatable material to form a composite in the form of a ramlet, such as those used in reactors.

By spacing the thermal ballast, many inefficiencies in the prior art can be eliminated. for example,
At temperatures up to about 3000 G, which are most important when carrying out hydrogen recovery processes, heat is transferred by convection using the gas flow as the conduction and convection means where the R-lets or particles are in contact with each other. Heat conduction as a heat transfer mechanism has traditionally been relatively inefficient due to the small contact surface area and low thermal conductivity of the binder when looking at the overall spacing of many particles or pellets. Heat transfer by hydrogen convection is also inefficient because the gas flow paths are tortuous and the thermal mass of the gas within the gas stream is typically small. In the present invention, where the heat transfer path between the reactant particles and the ballast is short, the conduction and convection processes can be easily carried out and the reaction time can be shortened. This cannot be expected, for example, if the thermal ballast is external to the hydrogenatable material and is not in contact or intimately mixed with the latter, resulting in slow absorption and desorption rates.

One way to manufacture the composite material used in the invention, e.g. as pellets, is to include a thermal ballast material of metal, e.g. nickel, in the form of particles, each of which is only a small fraction of the pellet's volume. However, it is convenient. 2. Three Hydrogenations - Hypothesis After cycling the hydrogenatable material itself breaks down to a particle size of 2-3 microns, but each pellet can hydrogenate a significant number of particles, e.g. at least about 10 particles. The dimensions of the hydridable material itself used to form the pellets are not critical, as long as they contain suitable metal particles.

(Regarding the preferred range of the 21st button operation and the ramometer, the upper temperature limit for the method of the present invention is about 500°C. From trace amounts to about 70°C.
Hydrogen partial pressures in concentrations up to % by volume range from a lower limit of 0.1 atm (absolute) to an upper limit of 200 atm. As mentioned above, the operating temperature is a function of the inherent properties of the hydrogenatable material and the partial pressure of hydrogen in the feed gas. The upper limit of 500° C. is only a guideline; this temperature can only be used for all-metal pellets or pellets held together by a heat resistant resin such as polytetrafluoroethylene.

After completion of hydrogenation of the layer by extraction of hydrogen from the gas stream,
Prior to the desorption of hydrogen from the formation, it is advantageous to purge the hydrogen-free gas from the reactor containing the formation, for example by flushing with a gas stream, such as a hydrogen gas stream.

This method improves the purity of the product. Furthermore, after completion of the adsorption at relatively low pressures and before passing the gas stream through the bed, it is advantageous to pressurize the reactor containing the column to a substantial proportion of the pressure of the gas stream to be treated. be.

Pressurization is carried out using a gas stream from which hydrogen has been removed (t1
(page 422) is convenient.

Mg r Fe'l'11 C! aN1a l LaN
A wide variety of hydride-forming metals can be used, including i47 (and other AB6 alloys). Typical examples of metal hydrides include alloys consisting of at least two elements selected from the group consisting of iron, titanium, nickel, calcium, manganese, magnesium, and rare earth elements.

New Chassis, Wyckoff MPD Technol
FeTi and its variants F8o, 9Mo, 1Ti and Fe0.8Nio, ai, caN16 and its variants, Cao7Mo, aNio, a, Cao, a by OgyCorp, under the trademark HYS'rOH.
Mo, 5Ni5. MNl,5(CFM)Ni5,
LaNi5 and variants of lanthanum and mitshu metal materials,
LaNi47 A10-a and MNl4. a AJo,
Suitable materials are commercially available, such as alloys having the chemical formula a I MgaNi and Mg2C'u (M-Mitsumetal, cFM-Cerium-free Mitschmetal).

Various other hydride-forming metals are known and cited in the above-mentioned papers in the prior art relating to metal hydride-hydrogen separation processes and are referenced herein (page 23). Other specific hydride materials are disclosed in US Pat. No. 4,142,300, which is incorporated herein by reference.

In the absorption phase of the rapid cycling process of the present invention, T
The front end is formed by a 2-T process, where T2 is the highest temperature of the layer and T1 is the lowest temperature of the layer ahead of the front end. With proper selection of ballast and assembly as described above, the front end defined by the T2-T construction will be approximately 40
℃, preferably 50. 'C or more and no more than 10 feet in length, preferably no more than 3.5 feet in length. Moreover, when the ballast is incorporated with the proper spatial distribution as described above, the leading end will be at least 0.1 ft7, preferably 0.
．． Pass through the reactor at a rate of 35 ft7 minutes.

After the front end has passed through the entire length of the bed, the uptake of the hydridable substance is achieved and the supply to the bed is terminated.

Desorption of the layer then takes place by lowering the layer pressure. Normally, this point is the starting point P. homogeneous (±50%, preferably ±20%) from hydrogenatable materials
) pressure drop is adjusted to allow hydrogen desorption to occur at a rate of . This is determined based on experience. The purpose of the desorption reaction is to proceed approximately along @El"-A. If the pressure drop is too fast, sub-cooling will occur, slowing down the desorption rate. If the pressure drop is too slow,
Stored heat is not used properly to perform rapid desorption. When carried out in the absence of external ballasts or heat transfer means using metal-bonded composite hydride structures, e.g. pellets, the invention is characterized by a relatively high tolerance for sub-cooling. There is.

This does not mean that the hydrogen reactor equipment is not sub-cooled during desorption when using metal-bound hydride pellets, but rather that the heat transfer between the pellets is relatively good. Fast desorption usually means that no sub-cooling occurs.

The process of the present invention is normally used in an alternating circulation, multi-stage reactor apparatus such as that illustrated in FIG. Valve HtJ7J is alternately opened and closed as schematically shown, and the hydrogen-containing feed streams are respectively fed into the communicating reactor (+aH). If a is closed and valve Ql is open, the hydrogen-containing feed stream passes through the hydrogenation reactor 04) and the dehydrogenated exhaust gas leaving this reactor α passes through the open valve (II).
through the recirculation blower (2I (optional) or sent to the dehydrogenation stream removal tube (21). The gas from the recirculation blower (a) is recirculated and Further hydrogen extraction is carried out with the hydrogen feed stream.Reactor 0
When 4) is in hydrogenation mode, valve 0 is closed, the previously hydrogenated reactants in reactor ae are degassed by depressurization, and the released hydrogen passes through valve 0. and the recovered hydrogen stream.

At the end of the hydrogenation reaction in the reactor 04 and the dehydrogenation reaction in the reactor allil, the valve (2 hot water is closed and the reactor 0υ is set to P).

repressurized. Valve α (23) is then opened to begin the hydrogenation reaction in the next cycle of reactor Oe, while valve tilt 0 is closed and the valve holder is opened to allow desorption of the reactants in reactor Oe. At pressure, dehydrogenation and passage of the released hydrogen from the reactor (14) into the recovered hydrogen stream takes place. Temperatures of 100 F (37 C) and 177 F (80 C) are shown. Such process temperatures represent a hydrogen pressure and approx. -50 psia
(1.36 to 3.4 atmospheres absolute) is within the normal range of dehydrogenation pressures.

The following examples provide a detailed explanation of the invention.

Example 1 The population temperature is ω°C, 5 nickel lanthanum is used as the hydrogenatable substance, and the numbers showing the relationship between the hydrogen partial pressure and the equilibrium temperature are used to produce hydrogen at a pressure of 500 psia, The design of the system for separating hydrogen from ammonia-f-diges containing 20 g nitrogen, 11 g methane, 6 g argon and 3% ammonia is as follows: Based on the data, the inlet hydrogen partial pressure is 30
0 psia, and the design desorption pressure is 30 psia. The equilibrium temperature limits in this case are 92°C and 24'C. Therefore, during absorption, a temperature increase of 68 degrees Celsius occurs in 5 nickel lanthanum.

(127j.

It is possible to absorb ioo@ of reaction heat during absorption, and 10
When the composite pellet absorbs 0% heat and uses this heat for desorption, it is nickel powder (325 mesh).
It is designed on the assumption that it is combined with granular 5 nickel lanthanum (325 mesh). Nickel powder is 5
The particle size is within ±50 inches of the particle size of nickel lanthanum. The design energy criteria for the composite are as follows: (a) Heat of reaction: (b) Heat capacity of LaNi5; (c) Heat capacity of nickel: ia + heat capacity of H2; It is not used because it is a sintered pellet used as a binder.

Based on 100 grams of 5-nickel lanthanum, the design pellets are 18.3% 5-nickel lanthanum and 81.7%
% of nickel. From an energy perspective,
Although the amount of larger sized nickel powder is the same, such larger size particles are less likely to be sufficient to achieve the desired short reaction fronts and fast reaction front velocities necessary to obtain commercially desirable cycle times. Does not necessarily provide heat transfer.

To obtain a suitable reaction front as designed by Ta T I have to. For example, even if the composite is properly designed, a flow rate that is too high may place too much stress on the composite. Rather, it is advantageous to lower the flow rate than the capacity of the composite. In many cases, reaction front lengths of 1-4 feet are used.

Example 2 A series of hydrogen separations was carried out using a gas mixture of 50% hydrogen and Yu Seki's methane (by volume) as the feed for Experiments 1-4. The feed for subsequent experiments was ammonia! as described in Example 1. -It was Jigas. 24.3%
5 nickel lanterns (325 mesh US standard),
72.8% nickel powder (80 (page 29) mesh US standard) and 2.9 lbs of silicone rubber (SO
Composite pellets of 1/2 were made using an initial composition consisting of 1/2 (by weight) (by weight). Pellets were made by mixing the above amounts of ingredients and forming a hydrogen permeable composite cylinder on a Carper press using standard KBR tablet dye. The cylinder formed was 1 inch in diameter and 114 inches long and then carved.

Sintered LaNi51 nickel ballasted pellets were prepared by mixing LaN1a (25%) and nickel powder sold under the trade name In□o123 and pressing into pellet form. The pellets were sintered at 1400F for minutes under flowing argon. After sintering, the pellets were crushed and sieved to a -4 to +1O mesh US standard size. Other composites of the type described were prepared in a manner similar to that described above, in a conventional manner or as described in Example 1.

A 5 foot, 3/4 inch insulated tubular reactor with an internal diameter of 0.68 inches was filled with approximately 1,000 grams of composite pellets. After charging, the column is prepressurized to 500 psia with methane to minimize pressure during feed introduction (page 30). After prepressurization, the feed is introduced into the bottom of the reactor at 500 psia. The effluent gas from the reactor was monitored and the front length was calculated by dividing the time required from feed introduction until hydrogen exits the reactor by the surface velocity of the feed gas. Table 1 provides a summary of several experiments and pellet configurations using the feed gases described above.

(Page 33) According to the data in Table 1, the breakthrough front end length Lf is the front end speed ■
It is proportional to the gyuto of f, that is, 1. It can be seen that fOCVf%.

Comparing the performance of the pellet formulations displayed in Table 1, all metals, sintered pellets (Experiments 14-18
) is easily seen to have excellent breakthrough characteristics. This result is obtained for the following reasons: (1) heat transfer between pellets is improved due to closer hydride/ballast contact; The polyethylene fills the R-let pores to some extent, preventing H2 transport within the pellet.

However, the resin-bonded system was superior in that the reaction front Lf was short and f was large (for example, 0.4 or more).

The polyethylene bonded system performed the worst, which is believed to be due to pore blockage.

[Brief explanation of drawings]

FIG. 1 is a plot of the theoretical equilibrium curve for hydride-forming metals, a representative Iwao Saki plot of equilibrium pressure versus hydrogen capacity for hydride-forming metals, and FIG. FIG. 2 is a schematic diagram of a processing device used in a hospital. 10.12, 18, 22, 24. Ka…sweat, 14,
16...Reactor, addition...Recirculation blower. Special Pestle Applicant Air, Products, &. Chemicals, Inc. MBG, Technology. Corporation Page 1 continued ■ Inventor: Nidwin Snape 14 Unda Drive, Suffern, New York, 10901 USA 0 Inventor: Raymond Peter Stickle 536' Hajid Mill Road, Concord, Mass., 01742 USA 0 Author: Gorton Chan Lin Cheno 222, Carlisle Stony Gate, Massachusetts, USA 01741 @ Inventor: Ernest Gee Huston, Taxed Maple Prussian Box 38, New York, USA 10987 (Inventor: M.P.・G Technology Corporation 681 Rollins Road, Wickoff, New York, New York 07481 Procedural Amendment October 27, 1982 26 Name of Invention Method for Separating Hydrogen from Mixed Gas 4, Agent 3, Ginza, Chuo-ku, Tokyo -3-12 Ginza Building (561-
5386/0274) 8. Contents of amendment as attached.

Claims (1)

[Claims] (1) (a) The composite changes from the initial hydrogen pressure, hydrogen concentration, and temperature (pHc1+T1) to the final hydrogen pressure, hydrogen concentration, and temperature (P2 r C2+ 'ra), and P2 becomes Pl
bigger than. comprising a homogeneous composite of a material capable of being hydrogenated and an inert thermal ballast under conditions where C2 is greater than 01, C2-C1 constitutes at least 50% of the theoretical hydrogenation capacity, and T2 is greater than T□. passing a hydrogen-containing gas mixture through a layer containing said ballast in an amount such that said composite absorbs at least 50% of the theoretical energy of hydride formation; b) desorbing hydrogen from the layer by reducing the pressure and utilizing the hydride formation energy for desorption. (2) The above compound is used in a high cycle method (second
Page) A gas mixture according to claim 1, characterized in that it contains sufficient ballast to supply at least 90 g of the heat required to carry out the desorption of the hydrogenatable substance. A method for rapidly separating hydrogen from (3) a hydridable material, wherein the composite has at least two elements selected from the group consisting of iron, nickel, calcium, manganese, magnesium, titanium, and rare earth elements; A method for rapidly separating hydrogen from a mixed gas in a high cycle according to claim 1, characterized in that the pellets contain a metal powder as a ballast. (4) A patent characterized in that the double gas mixture is passed through the bed such that the length of the reaction front is no more than 6 feet and the front velocity is no less than 0.3 feet per minute. A method for rapidly separating hydrogen from a mixed gas in a high cycle according to claim (3). (5) The ratio of ballast to hydridable material in the pellet is approximately 150% from the theoretical ratio (3) (
(Page 3) A method for rapidly separating hydrogen from a mixed gas in a high cycle according to claim (4). (6) A method for rapidly separating hydrogen from a mixed gas in a high cycle according to claim (4), wherein the proportion of hydrogen in the mixed gas is from a trace amount to about 70 volumes. (7) The method for rapidly separating hydrogen from a mixed gas in a high cycle according to claim (3), wherein the pellet is a sintered pellet. (8) -! Before the stage of desorbing hydrogen from let,
Rapid separation of hydrogen from a gas mixture in a high cycle according to claim 3, characterized in that a gas stream is passed as a rinsing agent through the reactor containing the above-mentioned layers. how to. (9) According to claim (6), the desorption rate is adjusted so that the mass flow rate of hydrogen removed from the reactor during desorption does not exceed the earthen floor. A method for rapidly separating hydrogen from a mixed gas in a high cycle. (IG After the above desorption and before the introduction of the feed gas stream,
A method for rapidly separating hydrogen from a mixed gas in a high cycle according to claim 9, characterized in that the reactor is pressurized to the working pressure. (11) The method for rapidly separating hydrogen from a mixed gas in a high cycle according to claim (8), characterized in that the gas flow passing through the reactor as an IJ agent is a hydrogen gas flow. . 0 - The method for rapidly separating hydrogen from a mixed gas in a high cycle according to claim (8), wherein the absorption and desorption are performed in a multistage reactor.