Simultaneous shift-reactive and adsorptive process to produce hydrogen
원문보기
IPC분류정보
국가/구분
United States(US) Patent
등록
국제특허분류(IPC7판)
C01B-031/20
C01B-031/00
출원번호
US-0280843
(2002-10-25)
등록번호
US-7354562
(2008-04-08)
발명자
/ 주소
Ying,David Hon Sing
Nataraj,Shankar
Hufton,Jeffrey Raymond
Xu,Jianguo
Allam,Rodney John
Dulley,Sarah Jane
출원인 / 주소
Air Products and Chemicals, Inc.
대리인 / 주소
Hoke, Jr.,Bryan C.
인용정보
피인용 횟수 :
31인용 특허 :
17
초록▼
A process for producing a high temperature COx-lean product gas from a high temperature COx-containing feed gas, includes: providing a sorption enhanced reactor containing a first adsorbent, a shift catalyst and a second adsorbent; feeding into the reactor a feed gas containing H2, H2O, CO and CO2;
A process for producing a high temperature COx-lean product gas from a high temperature COx-containing feed gas, includes: providing a sorption enhanced reactor containing a first adsorbent, a shift catalyst and a second adsorbent; feeding into the reactor a feed gas containing H2, H2O, CO and CO2; contacting the feed gas with the first adsorbent to provide a CO2 depleted feed gas; contacting the CO2 depleted feed gas with the shift catalyst to form a product mixture comprising CO2 and H2; and contacting the product mixture with a mixture of second adsorbent and shift catalyst to produce the product gas, which contains at least 50 vol. % H2, and less than 5 combined vol. % of CO2 and CO. The adsorbent is a high temperature adsorbent for a Sorption Enhanced Reaction process, such as K2CO3 promoted hydrotalcites, modified double-layered hydroxides, spinels, modified spinels, and magnesium oxides.
대표청구항▼
The invention claimed is: 1. A process for producing a CONx-lean product gas from a COx-containing feed gas, said process comprising: providing a sorption enhanced reactor containing a first bed, an intermediate bed downstream of the first bed and a second bed downstream of the intermediate bed, an
The invention claimed is: 1. A process for producing a CONx-lean product gas from a COx-containing feed gas, said process comprising: providing a sorption enhanced reactor containing a first bed, an intermediate bed downstream of the first bed and a second bed downstream of the intermediate bed, and wherein the first bed contains a first adsorbent, the second bed contains a mixture of a second adsorbent and a shift catalyst, and the intermediate bed contains the shift catalyst; feeding the feed gas into the reactor at a feed gas pressure during a reaction step, wherein the feed gas comprises H2, H2O, CO and CO2; contacting the feed gas with the first adsorbent to adsorb an amount of CO2 from the feed gas and to provide a CO2 depleted feed gas; contacting the CO2 depleted feed gas with the shift catalyst to catalyze a shift reaction of CO and H2O to form a product mixture comprising CO2 and H2; contacting the product mixture with the mixture of the second adsorbent and the shift catalyst to produce the product gas, wherein the product gas comprises at least 50 vol. % H2 and less than 5 combined vol. % CO2 and CO; regenerating the first adsorbent and the second adsorbent; repressurizing the reactor with a pressurization gas; and countercurrently purging the reactor at the feed gas pressure with a purge gas before regenerating the first adsorbent and the second adsorbent to yield an effluent stream containing unreacted CO and H2O, and recycling the effluent stream to the feed gas. 2. The process of claim 1, wherein the first adsorbent and the second adsorbent are independently at least one member selected from the group consisting of: (a) K2 CO3 promoted hydrotalcites; (b) modified double layered hydroxides represented by Formula I: description="In-line Formulae" end="lead"(Mg(1-x)AlX(OH)2)(CO3) x/2yH2OzM12CO3tm (I)description="In-line Formulae" end="tail" where 0.09≦x≦0.40, 0 ≦y≦3.5, 0≦z≦3.5, and M1 is Na or K; (c) spinels and modified spinels represented by Formula II: description="In-line Formulae" end="lead"Mg(A12)04yK2CO3tm (II)description="In-line Formulae" end="tail" where 0≦y≦3.5; and (d) magnesium oxide-containing adsorbents represented by Formula Ill: description="In-line Formulae" end="lead"{(M2CO3)m(2MHCO3)(1-im)}n(MgCO3)p(MgO)(1-p)xH2 O tm (Ill)description="In-line Formulae" end="tail" where M is an alkali metal, 0≦m ≦1, 0≦n ≦1.3, 0≦p 2 removal of {MgCO3}y {Mg(OH)2}(1-y)xH2, O in which 0.1 ≦y ≦0.9, and x indicates an extent of hydration. 3. The process of claim 1, wherein the feed gas is a syngas effluent from a high temperature shift reactor, and a raw syngas to the high temperature shift reactor is obtained from a steam methane reformer, partial oxidation reactor, air-blown autothermal reformer or oxygen-blown autothermal reformer upstream of the reactor. 4. The process of claim 1, wherein the feed gas is fed into the reactor at a flow rate of 5-50 gmole/hr/cm2 and a reactor temperature during the process is maintained between 175�� C. and 550�� C. 5. The process of claim 1, wherein the purge gas comprises at least one of steam and a steam/H2 mixture. 6. The process of claim 1, wherein the process is conducted in a series of cycles in more than one said reactor, and a first reactor is being regenerated while a second reactor is being operated in parallel to produce the product gas. 7. A process for producing a COx-lean product gas from a COx-containing feed gas, said process comprising: providing a sorption enhanced reactor containing a first bed, an intermediate bed downstream of the first bed and a second bed downstream of the intermediate bed, and wherein the first bed contains a first adsorbent, the second bed contains a mixture of a second adsorbent and a shift catalyst, and the intermediate bed contains the shift catalyst; feeding the feed gas into the reactor at a feed gas pressure during a reaction step wherein the feed gas comprises H2, H2O, CO and CO2; contacting the feed gas with the first adsorbent to adsorb an amount of CO2 from the feed gas and to provide a CO2 depleted feed gas; contacting the CO2 depleted feed gas with the shift catalyst to catalyze a shift reaction of CO and H2 O to form a Product mixture comprising CO2 and H2: contacting the Product mixture with the mixture of the second adsorbent and the shift catalyst to Produce the product gas, wherein the product gas comprises at least 50 vol. % H2 and less than 5 combined vol. % CO2 and CO; regenerating the first adsorbent and the second adsorbent; repressurizing the reactor with a pressurization gas; and cocurrently rinsing the reactor at the feed gas pressure with a CO2 product before regenerating the first adsorbent and the second adsorbent and recovering a CO2-rich byproduct stream during the regenerating step. 8. The process of claim 7, wherein the first adsorbent and the second adsorbent are independently at least one member selected from the group consisting of: (a) K2CO3 promoted hydrotalcites; (b) modified double layered hydroxides represented by Formula I: description="In-line Formulae" end="lead"(Mg(1-X)Alx(OH)2)(CO3) x/2yH2OzM12 CO3tm (I)description="In-line Formulae" end="tail" where 0.09≦x ≦0.40, 0 ≦y ≦3.5, 0 ≦z ≦3.5, and Ml is Na or K; (c) spinels and modified spinels represented by Formula II: description="In-line Formulae" end="lead"Mg(Al2)O4yK2 CO3tm (II)description="In-line Formulae" end="tail" where 0 ≦y ≦3.5; and (d) magnesium oxide-containing adsorbents represented by Formula Ill: description="In-line Formulae" end="lead"{(M2CO3)m(2MHCO3)(1-m) }n(MgCO3)p(MgO)(1-p)xH2O tm (Ill)description="In-line Formulae" end="tail" where M is an alkali metal, 0≦m ≦1, 0≦n ≦1.3, 0≦p 2 removal of {MgCO3)y{Mg(OH)2}(1-y)xH2 O, in which 0.1≦y≦0.9, and x indicates an extent of hydration. 9. The process of claim 7, wherein the feed gas is a syngas effluent from a high temperature shift reactor, and a raw syngas to the high temperature shift reactor is obtained from a steam methane reformer, partial oxidation reactor, air-blown autothermal reformer or oxygen-blown autothermal reformer upstream of the reactor. 10. The process of claim 7, wherein the feed gas is fed into the reactor at a flow rate of 5-50 gmole/hr/cm2 and a reactor temperature during the process is maintained between 1750�� C. and 550�� C. 11. The process of claim 7, wherein the process is conducted in a series of cycles in more than one said reactor, and a first reactor is being regenerated while a second reactor is being operated in parallel to produce the product gas.
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