A cyclic process for selectively separating hydrogen sulfide from a gas mixture including CO2 is operated by contacting the gas mixture under sorption conditions with a non-aqueous sorbent comprising a basic non-protogenic nitrogenous compound to react the H2S with the basic compound so that the H2S
A cyclic process for selectively separating hydrogen sulfide from a gas mixture including CO2 is operated by contacting the gas mixture under sorption conditions with a non-aqueous sorbent comprising a basic non-protogenic nitrogenous compound to react the H2S with the basic compound so that the H2S can be sorbed by the compound. The compound containing the sorbed H2S can then be subjected to desorption conditions by which the H2S is desorbed and the sorbent readied for another sorption step in the cycle. The basic nitrogenous compound can be carried on a porous solid sorbent, e.g., a solid oxide such as alumina, silica, silica-alumina, zeolites, or a mesoporous and/or macroporous solid oxide. The process may be operated using a pressure swing, temperature swing, partial pressure swing, purge displacement, or a combination thereof between the sorption and desorption portions of the cycle, preferably in a rapid cycle operation.
대표청구항▼
1. A cyclic process for selectively separating H2S from a feed gas mixture comprising CO2 and H2S, which process comprises: a) contacting the feed gas mixture under sorption conditions with a non-aqueous sorbent comprising a basic non-protogenic, tertiaryaminosiloxane compound grafted onto a mesopor
1. A cyclic process for selectively separating H2S from a feed gas mixture comprising CO2 and H2S, which process comprises: a) contacting the feed gas mixture under sorption conditions with a non-aqueous sorbent comprising a basic non-protogenic, tertiaryaminosiloxane compound grafted onto a mesoporous solid oxide having surface silanol groups selected from MCM-41, MCM-48, SBA-1, SBA-2, SBA-3, SBA-15, KIT-1, KIT-5, KIT-6, and combinations thereof, which sorbent reacts with at least a portion of the H2S in the feed gas mixture;b) sorbing the H2S and some of the CO2 onto the adsorbent, wherein the nonaqueous adsorbent has a selectivity for H2S over CO2 under the adsorption conditions;c) subjecting the adsorbent to desorption conditions by which at least a portion of the sorbed H2S is desorbed; andd) retrieving an H2S-rich product stream that has a higher mol % of H2S than the feed gas mixture. 2. A process according to claim 1 in which the sorption and desorption steps are conducted at different pressures wherein the total pressure of the desorption step is lower than the total pressure of the sorption step. 3. A process according to claim 1 in which the sorption and desorption steps are conducted at different pressures wherein the partial pressure of H2S in the desorption step is less than the partial pressure of H2S in the sorption step. 4. A process according to claim 1 in which the sorption and desorption steps are conducted at different temperatures. 5. A process according to claim 1 in which at least a portion of the sorbed H2S is desorbed by a non-sorbing inert purge gas and/or by a displacement purge gas. 6. A process according to claim 2 in which desorption is carried out in at least two steps under conditions of different pressure in each step with the pressure of the first desorption step being higher than the pressure of the second desorption step so that most of the CO2 adsorbed in the adsorption step is desorbed in the first desorption step and most of the H2S adsorbed in the adsorption step is desorbed in the second desorption step. 7. A process according to claim 1 in which the process is operated cyclically between the adsorption and desorption conditions with a total cycle time of less than one minute. 8. A process to claim 1 in which the CO2 and H2S partial pressures during the adsorption step are less than about 1 bar. 9. A process to claim 1 in which the feed gas mixture contains less than 5 mol % water. 10. A cyclic process for selectively separating H2S from a natural gas feed stream comprising H2S and CO2, which process comprises: (i) contacting the natural gas feed stream under H2S adsorption conditions with a non-aqueous adsorbent comprising a basic non-protogenic, tertiaryaminosiloxane compound grafted onto a mesoporous solid oxide having surface silanol groups selected from MCM-41, MCM-48, SBA-1, SBA-2, SBA-3, SBA-15, KIT-1, KIT-5, KIT-6, and combinations thereof where in the non-aqueous adsorbent has a selectivity for H2S over CO2 under the conditions;(ii) reacting at least a portion of the H2S in the natural gas feed stream with the sorbent so that the H2S is absorbed by the adsorbent;(iii) retrieving a natural gas product stream having a lower content of H2S in mol % than the natural gas feed stream;(iv) subjecting the adsorbent containing the adsorbed H2S to desorption conditions by which at least a portion of the H2S in the sorbent is desorbed from the sorbent;(v) retrieving an H2S rich product stream that has a higher mol % of H2S than the natural gas feed stream;(vi) passing at least a portion of the H2S-rich product stream to a Claus plant; and(vii) recovering sulfur from the H2S in a side stream. 11. A process according to claim 10 wherein the natural gas feed stream contains from about 10 vppm to about 10,000 vppm H2S and wherein the natural gas product stream contains less than about 4 vppm H2S. 12. A process according to claim 11 wherein the natural gas feed stream contains at least 5 mol % CO2 and wherein the natural gas product stream contains at most 5 mol % less CO2 than the natural gas feed stream. 13. A process according to claim 11 in which the adsorption and desorption steps are conducted at different pressures, wherein (a) the total pressure of the desorption step is lower than the total pressure of the adsorption step, (b) the partial pressure of H2S in the desorption step is less than the partial pressure of H2S in the adsorption step, or (c) both (a) and (b). 14. A process according to claim 11 in which at least a portion of the sorbed H2S is desorbed by a non-sorbing inert purge gas and/or by a displacement purge gas. 15. A cyclic process for separating H2S and CO2 from a natural gas feed stream comprising H2S and CO2, from a producing formation, which process comprises: (i) contacting the natural gas feed stream under H2S adsorption conditions with a non-aqueous adsorbent comprising a basic non-protogenic tertiaryaminosiloxane compound grafted onto a mesoporous solid oxide having surface silanol groups selected from MCM-41, MCM-48, SBA-1, SBA-2, SBA-3, SBA-15, KIT-1, KIT-5, KIT-6, and combinations thereof wherein the non-aqueous adsorbent has a selectivity for H2S over CO2 under the H2S adsorption conditions;(ii) reacting at least a portion of the H2S and CO2 in the natural gas feed stream with the sorbent so that the H2S and the CO2 are adsorbed by the adsorbent;(iii) retrieving a natural gas product stream having a lower mol % of each H2S and CO2 than the natural as feed stream;(iv) subjecting the adsorbent containing the adsorbed H2S and CO2 to first desorption conditions by which a higher mol % of CO2 is desorbed than H2S;(v) retrieving a CO2 rich product stream that has a higher mol % of CO2 than the natural gas feed stream;(vi) subjecting the adsorbent containing the adsorbed H2S and CO2 to second desorption conditions by which a higher mol % of H2S is desorbed than CO2;(vii) retrieving an H2S-rich product stream that has a higher mol % of H2S than the natural gas feed stream; and(viii) re-injecting the side stream comprising CO2 into the producing formation. 16. A process according to claim 15 further comprising: sending at least a portion of the H2S-rich stream to a Claus plant; andrecovering sulfur from the H2S-rich stream. 17. A cyclic process for separating H2S and CO2 from a feed gas stream comprising H2S and CO2, to produce a first product gas stream comprising H2S and a second product gas stream comprising CO2 depleted in H2S, which process comprises: (i) contacting the feed gas stream under H2S adsorption conditions with a non-aqueous adsorbent comprising a basic non-protogenic tertiaryaminosiloxane compound grafted onto a mesoporous solid oxide having surface silanol groups selected from MCM-41, MCM-48, SBA-1, SBA-2, SBA-3, SBA-15, KIT-1, KIT-5, KIT-6, and combinations thereof wherein the non-aqueous adsorbent has a selectivity for H2S over CO2 under the H2S adsorption conditions;(ii) reacting at least a portion of the H2S and the CO2 in the feed gas stream with the adsorbent so that the H2S and CO2 are adsorbed by the adsorbent;(iii) subjecting the adsorbent containing the adsorbed H2S and CO2 to CO2 desorption conditions by which a higher mol % of the CO2 is desorbed than H2S;(iv) retrieving a CO2 rich product stream that has a higher mol % of CO2 than the feed gas stream;(v) subjecting the adsorbent containing the adsorbed H2S and CO2 to H2S desorption conditions by which a higher mol % of H2S is desorbed than CO2; and(vi) retrieving an H2S rich product stream that has a higher mol % of H2S than the feed gas stream. 18. A process according to claim 17 in which the CO2 rich product stream has a lower mol % of H2S than the feed gas stream. 19. A process according to claim 18 in which the feed gas stream comprises at least a combined total of 50 mol % H2S and CO2, wherein the feed gas stream is a pre-separated contaminant stream resulting from the separation of H2S and CO2 from a natural gas stream from a producing formation and the CO2-rich stream is re-injected into the producing formation. 20. A process according to claim 17 in which at least a portion of the H2S-rich product stream is passed to a Claus plant for the recovery of sulfur.
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