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While significant advancements have been achieved in separating H\n                    <jats:sub>2<\/jats:sub>\n                    S from CH\n                    <jats:sub>4<\/jats:sub>\n                    , the selective removal of H\n                    <jats:sub>2<\/jats:sub>\n                    S from CO\n                    <jats:sub>2<\/jats:sub>\n                    remains a formidable challenge due to their similar physicochemical properties. Herein, we report a breakthrough strategy utilizing reversible nucleophilic addition reaction between carbonyl group and H\n                    <jats:sub>2<\/jats:sub>\n                    S, departing from conventional acid\u2010base interaction\u2010based liquid\u2010phase capture processes. Through comprehensive characterization using nuclear magnetic resonance (NMR) and Fourier transform infrared (FT\u2010IR) spectroscopy, we confirmed the formation of nucleophilic addition products between the designed carbonyl\u2010functionalized ionic liquids (ILs) and H\n                    <jats:sub>2<\/jats:sub>\n                    S. Dispersion\u2010corrected DFT calculations revealed that the nucleophilic addition products facilitate secondary H\n                    <jats:sub>2<\/jats:sub>\n                    S capture through two distinct approaches: 1) conformational matching and 2) dissociation of H\n                    <jats:sub>2<\/jats:sub>\n                    S into [HS]\u207b species. The unique cascade H\n                    <jats:sub>2<\/jats:sub>\n                    S sorption mechanism demonstrates exceptional affinity for H\n                    <jats:sub>2<\/jats:sub>\n                    S, endowing the [6ca]\u2010derived ILs with unprecedented high H\n                    <jats:sub>2<\/jats:sub>\n                    S capacities and record\u2010breaking H\n                    <jats:sub>2<\/jats:sub>\n                    S\/CO\n                    <jats:sub>2<\/jats:sub>\n                    selectivities (67\u201389 at 1.0\u00a0bar and 229\u2013319 at 0.1\u00a0bar), surpassing previously reported values. Combined with energy\u2010efficient regeneration cycles, these findings establish a new paradigm for H\n                    <jats:sub>2<\/jats:sub>\n                    S\/CO\n                    <jats:sub>2<\/jats:sub>\n                    separation with significant potential for natural gas valorization.\n                  <\/jats:p>","DOI":"10.1002\/anie.202504337","type":"journal-article","created":{"date-parts":[[2025,7,24]],"date-time":"2025-07-24T07:02:18Z","timestamp":1753340538000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":19,"title":["Efficient Hydrogen Sulfide Separation from Carbon Dioxide Achieved by Carbonyl\u2010Functionalized Ionic Liquids for Natural Gas Upgrading"],"prefix":"10.1002","volume":"64","author":[{"given":"Mingzhen","family":"Shi","sequence":"first","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical Engineering Nanjing University  Nanjing 210023 P.R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuhua","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical Engineering Nanjing University  Nanjing 210023 P.R. China"},{"name":"State Key Laboratory of Coordination Chemistry, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices The Institute of Green Chemistry and Engineering School of Chemistry and Chemical Engineering Nanjing University  Jiangsu 215163 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Youting","family":"Wu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical Engineering Nanjing University  Nanjing 210023 P.R. 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