IPC분류정보
국가/구분 |
United States(US) Patent
등록
|
국제특허분류(IPC7판) |
|
출원번호 |
US-0570346
(2009-09-30)
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등록번호 |
US-8303930
(2012-11-06)
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발명자
/ 주소 |
|
출원인 / 주소 |
- American Air Liquide, Inc.
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대리인 / 주소 |
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인용정보 |
피인용 횟수 :
3 인용 특허 :
11 |
초록
▼
The present invention relates to various processes for recovering high purity gaseous hydrogen and high purity gaseous carbon dioxide from the gas stream produced using steam hydrocarbon reforming, especially steam methane reforming, utilizing a H2 pressure swing adsorption unit followed by either a
The present invention relates to various processes for recovering high purity gaseous hydrogen and high purity gaseous carbon dioxide from the gas stream produced using steam hydrocarbon reforming, especially steam methane reforming, utilizing a H2 pressure swing adsorption unit followed by either a CO2 vacuum swing adsorption unit or a CO2 vacuum swing adsorption unit in combination with an additional CO2 pressure swing adsorption unit. By using an uncoupled H2 PSA and CO2 VSA unit it is possible to produce high purity H2 and high purity CO2. The present invention further relates to a process for optimizing the recovery of CO2 from waste gas streams produced during the hydrogen purification step of a steam hydrocarbon reforming/H2 pressure swing adsorption unit utilizing either a CO2 vacuum swing adsorption unit or a CO2 vacuum swing adsorption unit in combination with a CO2 pressure swing adsorption unit. The present invention even further relates to the apparatus necessary to carry out the various processes of the present invention.
대표청구항
▼
1. A process for recovering high purity gaseous hydrogen and high purity gaseous carbon dioxide, the process comprising the steps of: a) generating a hydrogen rich effluent that also contains carbon monoxide, carbon dioxide, methane and water from one or more hydrocarbon feed gases in a steam hydroc
1. A process for recovering high purity gaseous hydrogen and high purity gaseous carbon dioxide, the process comprising the steps of: a) generating a hydrogen rich effluent that also contains carbon monoxide, carbon dioxide, methane and water from one or more hydrocarbon feed gases in a steam hydrocarbon reformer;b) treating the hydrogen rich effluent in a water gas shift reactor in order to further enrich the hydrogen rich effluent and also increase the carbon dioxide content in the hydrogen rich effluent thereby obtaining a water shift effluent, wherein said water shift effluent has a temperature of less than 50C and a pressure of between 200 psig and 600 psig;c) introducing the water shift effluent into a hydrogen pressure swing adsorption unit having two or more beds that contain one or more adsorbents that allow for the recovery of a high purity gaseous hydrogen stream and the adsorption of carbon dioxide, carbon monoxide, methane, water and the remaining hydrogen onto the adsorbents in the two or more beds;d) withdrawing the high purity gaseous hydrogen from the hydrogen pressure swing adsorption unit and passing this stream on for further use;e) depressurizing the two or more beds that contain the adsorbent in order to release the carbon dioxide, carbon monoxide, methane, water and the remaining hydrogen adsorbed thereto and produce a hydrogen pressure swing adsorption tail gas;f) withdrawing the hydrogen pressure swing adsorption tail gas from the hydrogen pressure swing adsorption unit and with the aid of a blower and introducing the hydrogen pressure swing adsorption tail gas into a vacuum swing adsorption unit that contains one or more beds of an adsorbent selected from zeolites, silica gels, activated alumina or mixtures thereof that are selective for carbon dioxide thereby allowing for the recovery of a high purity gaseous carbon dioxide by adsorption to the adsorbent and a first carbon dioxide lean gas stream that contains methane, hydrogen, carbon monoxide and the remaining carbon dioxide;g) allowing the first carbon dioxide lean gas stream to pass from the vacuum swing adsorption unit where it is recycled to the steam hydrocarbon reformer where it can used as makeup fuel gas in the steam hydrocarbon reformer; andh) vacuum desorbing the carbon dioxide from the adsorbent in the vacuum swing adsorption unit in order to produce a high purity gaseous carbon dioxide stream that may be passed on for further use. 2. The process of claim 1, wherein the blower of step f) is positioned after the VSA unit and aids in pulling the hydrogen pressure swing adsorption tail gas through the VSA unit. 3. The process of claim 1, wherein the blower of step f) is positioned before the VSA unit and aids in introducing the hydrogen pressure swing adsorption tail gas into the VSA unit. 4. A process for treating a hydrogen pressure swing adsorption tail gas stream that contains hydrogen, carbon monoxide, carbon dioxide, methane and water in order to recover high purity carbon dioxide from the tail gas stream, said process comprising the steps of: a) introducing the hydrogen pressure swing adsorption tail gas with the aid of a blower into a vacuum swing adsorption unit that contains one or more beds of an adsorbent that is selected from zeolites, silica gels, activated alumina and mixtures thereof that are selective for carbon dioxide thereby allowing for the recovery of a high purity gaseous carbon dioxide by adsorption of a large portion of the carbon dioxide to the adsorbent and a first carbon dioxide lean gas stream that contains methane, hydrogen, carbon monoxide and the remaining carbon dioxide;b) allowing the first carbon dioxide lean gas stream to pass from the vacuum swing adsorption unit where it is recycled for use as a makeup fuel; andc) vacuum desorbing the carbon dioxide from the adsorbent in the vacuum swing adsorption unit in order to produce a high purity gaseous carbon dioxide stream, wherein the feed to the hydrogen pressure swing adsorber has a temperature of less than 50C and a pressure of between 200 psiq and 600 psiq. 5. The process of claim 4, wherein the blower of step a) is positioned after the VSA unit and aids in pulling the hydrogen pressure swing adsorption tail gas through the VSA unit. 6. The process of claim 4, wherein the blower of step a) is positioned before the VSA unit and aids in introducing the hydrogen pressure swing adsorption tail gas into the VSA unit. 7. The process of claim 4, wherein the adsorbent is a zeolite that is a molecular sieve adsorbent. 8. The process of claim 7, wherein the molecular sieve adsorbent is 13X zeolite. 9. A process for recovering high purity gaseous hydrogen and high purity gaseous carbon dioxide, the process comprising the steps of: a) generating a hydrogen rich effluent that also contains carbon monoxide, carbon dioxide, methane and water from one or more hydrocarbon feed gases in a steam hydrocarbon reformer;b) treating the hydrogen rich effluent in a water gas shift reactor in order to further enrich the hydrogen rich effluent and also increase the carbon dioxide content in the hydrogen rich effluent thereby obtaining a water shift effluent, wherein said water shift effluent has a temperature of less than 50C and a pressure of between 200 psiq and 600 psiq;c) introducing the water shift effluent into a hydrogen pressure swing adsorption unit having two or more beds that contain one or more adsorbents that allow for the recovery of a high purity gaseous hydrogen stream and the adsorption of carbon dioxide, carbon monoxide, methane, water and the remaining hydrogen onto the adsorbents in the two or more beds;d) withdrawing the high purity gaseous hydrogen from the hydrogen pressure swing adsorption unit and passing this stream on for further use;e) depressurizing the two or more beds of the hydrogen pressure swing adsorption unit that contain the adsorbent in order to release the carbon dioxide, carbon monoxide, methane, water and the remaining hydrogen adsorbed thereto and produce a hydrogen pressure swing adsorption tail gas;f) withdrawing the hydrogen pressure swing adsorption tail gas from the hydrogen swing adsorption unit and introducing the hydrogen pressure swing adsorption tail gas into a vacuum swing adsorption unit that contains two or more beds of an adsorbent selected from zeolites, silica gels, activated aluminas and mixtures thereof that are selective for carbon dioxide thereby allowing for the recovery of a high purity gaseous carbon dioxide by adsorption to the adsorbent and a first carbon dioxide lean gas stream that contains methane, hydrogen, carbon monoxide and the remaining carbon dioxide;g) allowing the first carbon dioxide lean gas stream to pass from the vacuum swing adsorption unit to a compressor where the first carbon dioxide lean gas stream is compressed to a pressure that is higher than the pressure of the steam hydrocarbon reformer before being fed to a secondary pressure swing adsorption unit that contains two more beds that include activated carbon thereby allowing for the production of a secondary high purity hydrogen stream and a secondary pressure swing adsorption tail gas;h) vacuum desorbing the carbon dioxide from the adsorbent in the vacuum swing adsorption unit in order to produce a high purity gaseous carbon dioxide rich stream;i) withdrawing the high purity hydrogen stream from the secondary pressure swing adsorption unit and recycling the high purity hydrogen stream to either the feed gas of the steam hydrocarbon reformer, the hydrogen rich effluent that is withdrawn from the steam hydrocarbon reformer to be injected into the water gas shift reactor, or the water shift effluent to be injected into the hydrogen pressure swing adsorption unit;j) depressurizing the two or more beds of the secondary pressure swing adsorption unit to allow for the withdrawal of the secondary pressure swing adsorption tail gas; andk) recycling the secondary pressure swing adsorption tail gas to the steam hydrocarbon reformer as makeup fuel or to the hydrogen pressure swing adsorption tail gas stream to be injected into the carbon dioxide vacuum swing adsorption unit. 10. A process for treating a hydrogen pressure swing adsorption tail gas stream that contains hydrogen, carbon monoxide, carbon dioxide, methane and water in order to recover high purity carbon dioxide from the tail gas stream, said process comprising the steps of: a) introducing the hydrogen pressure swing adsorption tail gas into a vacuum swing adsorption unit that contains two or more beds of an adsorbent selected from zeolites, silica gels, activated aluminas and mixtures thereof that are selective for carbon dioxide thereby allowing for the recovery of a high purity gaseous carbon dioxide by adsorption to the adsorbent and a first carbon dioxide lean gas stream that contains methane, hydrogen, carbon monoxide and the remaining carbon dioxide;b) allowing the first carbon dioxide lean gas stream to pass from the vacuum swing adsorption unit to a compressor where the first carbon dioxide lean gas stream is compressed to a pressure that is higher than the pressure of the steam hydrocarbon reformer before being fed to a secondary pressure swing adsorption unit that contains two more beds that include activated carbon thereby allowing for the production of a secondary high purity hydrogen stream and a secondary pressure swing adsorption tail gas;c) vacuum desorbing the carbon dioxide from the adsorbent in the vacuum swing adsorption unit in order to produce a high purity gaseous carbon dioxide rich stream;d) withdrawing the high purity hydrogen stream from the secondary pressure swing adsorption unit and recycling the high purity hydrogen stream to either the feed gas of the steam hydrocarbon reformer, the hydrogen rich effluent that is withdrawn from the steam hydrocarbon reformer and injected into the water gas shift reactor, or the water shift effluent to be injected into the hydrogen pressure swing adsorption unit;e) depressurizing the two or more beds of the secondary pressure swing adsorption unit to allow for the withdrawal of the secondary pressure swing adsorption tail gas; andf) recycling the secondary pressure swing adsorption tail gas to the steam hydrocarbon reformer as makeup fuel or to the hydrogen pressure swing adsorption tail gas stream to be injected into the carbon dioxide vacuum swing adsorption unit, wherein the feed to the hydrogen pressure swing adsorber has a temperature of less than 50C and a pressure of between 200 psig and 600 psig. 11. A system for recovering high purity gaseous hydrogen and high purity gaseous carbon dioxide, the system comprising: a) a steam hydrocarbon reformer that generates a hydrogen rich effluent that also contains carbon monoxide, carbon dioxide, methane and water from one or more hydrocarbon feed gases;b) a water gas shift reactor for treating the hydrogen rich effluent to convert the carbon monoxide present in the hydrogen rich effluent to carbon dioxide to obtain a water shift effluent and a means for passing the hydrogen rich effluent from the steam hydrocarbon reformer to the water gas shift reactor, wherein said water shift effluent has a temperature of less than 50C and a pressure of between 200 psig and 600 psig;c) a hydrogen pressure swing adsorption unit having two or more beds that contain one or more adsorbents that allow for the recovery of a high purity gaseous hydrogen stream and a hydrogen pressure swing adsorption tail gas that contains the carbon dioxide, carbon monoxide, methane, water and the remaining hydrogen from the water shift effluent of the water gas shift reactor and a means for passing the water shift effluent from the water gas shift reactor to the hydrogen pressure swing adsorption unit;d) a vacuum swing adsorption unit that contains one or more beds of an adsorbent selected from zeolites, silica gels, activated aluminas and mixtures thereof that are selective for carbon dioxide thereby allowing for the recovery of a high purity gaseous carbon dioxide by adsorption to the adsorbent and a first carbon dioxide lean gas stream that contains methane, hydrogen, carbon monoxide and the remaining carbon dioxide and a means for passing the hydrogen pressure swing adsorption tail gas that contains the carbon dioxide, carbon monoxide, methane, water and the remaining hydrogen from the hydrogen pressure swing adsorption unit to the vacuum swing adsorption unit and a means for withdrawing the high purity gaseous hydrogen stream from the two or more beds that contain one or more adsorbents of the hydrogen pressure swing adsorption unit; ande) a means for recycling the first carbon dioxide lean gas stream to pass from the vacuum swing adsorption unit to the steam hydrocarbon reformer where it can be added to natural gas in order to fuel the steam hydrocarbon reformer and a means for desorbing the carbon dioxide from the adsorbent in the vacuum swing adsorption unit in order to produce a high purity gaseous carbon dioxide stream. 12. The system of claim 11, wherein the various means for passing include lines that allow for the passage of the gases and various optional pumps and blowers which assist in the movement of the gases from one point to another. 13. A system for recovering high purity gaseous hydrogen and high purity gaseous carbon dioxide comprising: a) a steam hydrocarbon reformer that generates a hydrogen rich effluent that also contains carbon monoxide, carbon dioxide, methane and water from one or more hydrocarbon feed gases;b) a water gas shift reactor for treating the hydrogen rich effluent to convert the carbon monoxide present in the hydrogen rich effluent to carbon dioxide to obtain a water shift effluent and a means for passing the hydrogen rich effluent from the steam hydrogen carbon reformer to the water gas shift reactor, wherein said water shift effluent has a temperature of less than 50C and a pressure of between 200 psig and 600 psiq;c) a hydrogen pressure swing adsorption unit having two or more beds that contain one or more adsorbents that allow for the recovery of a high purity gaseous hydrogen stream and a hydrogen pressure swing adsorption tail gas that contains the carbon dioxide, carbon monoxide, methane, water and the remaining hydrogen from the water shift effluent of the water gas shift reactor and a means for passing the water shift effluent from the water gas shift reactor to the hydrogen pressure swing adsorption unit;d) a vacuum swing adsorption unit that contains one or more beds of an adsorbent selected from zeolites, silica gels, activated aluminas and mixtures thereof that are selective for carbon dioxide thereby allowing for the recovery of a high purity gaseous carbon dioxide by adsorption to the adsorbent and a first carbon dioxide lean gas stream that contains methane, hydrogen, carbon monoxide and the remaining carbon dioxide and a means for passing the hydrogen pressure swing adsorption tail gas that contains the carbon dioxide, carbon monoxide, methane, water and the remaining hydrogen from the hydrogen pressure swing adsorption unit to the vacuum swing adsorption unit and a means for withdrawing the high purity gaseous hydrogen stream from the hydrogen pressure swing adsorption unit;e) a compressor for compressing the first carbon dioxide lean gas stream from the vacuum swing adsorption unit and a means for passing the first carbon dioxide lean gas stream from the vacuum swing adsorption unit to the compressor;f) a secondary pressure swing adsorption unit that contains one or more beds that include activated carbon thereby allowing for the production of a secondary high purity hydrogen stream and a secondary pressure swing adsorption tail gas and a means to pass the compressed first carbon dioxide lean gas stream form the compressor to the secondary pressure swing adsorption unit;g) a means to withdraw the high purity hydrogen stream from the secondary pressure swing adsorption unit and recycling the high purity hydrogen stream to either feed stream for the steam hydrocarbon reformer, the water gas shift reactor, or the hydrogen pressure swing adsorption unit; andi) a means to depressurize the two or more beds of the secondary pressure swing adsorption unit to allow for the withdrawal of the secondary pressure swing adsorption tail gas and a means for recycling the secondary pressure swing adsorption tail gas to be used with natural gas as fuel for the steam hydrocarbon reformer, to the water gas shift reactor or to be included in the water gas shift effluent. 14. The system of claim 13, wherein the various means for passing include lines that allow for the passage of the gases and various optional pumps and blowers which assist in the movement of the gases from one point to another.
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