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Their modular nature makes them amenable to crystal engineering studies, which have thus far afforded four HUM platforms (as classified by the inorganic linkers). HUMs are of practical interest because of their benchmark gas separation performance for several industrial gas mixtures. We report herein design and gram\u2010scale synthesis of the prototypal sulfate\u2010linked HUM, the\n                    <jats:bold>fsc<\/jats:bold>\n                    topology coordination network (\n                    <jats:bold>\n                      [Zn(tepb)(SO\n                      <jats:sub>4<\/jats:sub>\n                      )]\n                    <\/jats:bold>\n                    <jats:sub>\n                      <jats:italic>\n                        <jats:bold>n<\/jats:bold>\n                      <\/jats:italic>\n                    <\/jats:sub>\n                    ),\n                    <jats:bold>SOFOUR\u20101\u2010Zn<\/jats:bold>\n                    ,\n                    <jats:bold>tepb<\/jats:bold>\n                    =(tetra(4\u2010pyridyl)benzene). Alignment of the sulfate anions enables strong binding to C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    via O\u22c5\u22c5\u22c5HC interactions but weak CO\n                    <jats:sub>2<\/jats:sub>\n                    binding, affording a new benchmark for the difference between C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    and CO\n                    <jats:sub>2<\/jats:sub>\n                    heats of sorption at low loading (\u0394\n                    <jats:italic>Q<\/jats:italic>\n                    <jats:sub>st<\/jats:sub>\n                    =24\u2005kJ\u2009mol\n                    <jats:sup>\u22121<\/jats:sup>\n                    ). Dynamic column breakthrough studies afforded fuel\u2010grade C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    from trace (1\u2009:\u200999) or 1\u2009:\u20091\u2005C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    \/CO\n                    <jats:sub>2<\/jats:sub>\n                    mixtures, outperforming its SiF\n                    <jats:sub>6<\/jats:sub>\n                    <jats:sup>2\u2212<\/jats:sup>\n                    analogue,\n                    <jats:bold>SIFSIX\u201022\u2010Zn<\/jats:bold>\n                    .\n                  <\/jats:p>","DOI":"10.1002\/anie.202116145","type":"journal-article","created":{"date-parts":[[2021,12,20]],"date-time":"2021-12-20T12:59:08Z","timestamp":1640005148000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":65,"title":["The First Sulfate\u2010Pillared Hybrid Ultramicroporous Material, SOFOUR\u20101\u2010Zn, and Its Acetylene Capture Properties"],"prefix":"10.1002","volume":"61","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-4918-0730","authenticated-orcid":false,"given":"Debobroto","family":"Sensharma","sequence":"first","affiliation":[{"name":"Department of Chemical Sciences Bernal Institute University of Limerick  Limerick V94 T9PX Republic of Ireland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7105-3378","authenticated-orcid":false,"given":"Daniel J.","family":"O'Hearn","sequence":"additional","affiliation":[{"name":"Department of Chemical Sciences Bernal 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Ireland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5282-7304","authenticated-orcid":false,"given":"Naveen","family":"Kumar","sequence":"additional","affiliation":[{"name":"Department of Chemical Sciences Bernal Institute University of Limerick  Limerick V94 T9PX Republic of Ireland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3739-7489","authenticated-orcid":false,"given":"Benjamin H.","family":"Wilson","sequence":"additional","affiliation":[{"name":"Department of Chemical Sciences Bernal Institute University of Limerick  Limerick V94 T9PX Republic of Ireland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1592-0726","authenticated-orcid":false,"given":"Matthias","family":"Vandichel","sequence":"additional","affiliation":[{"name":"Department of Chemical Sciences Bernal Institute University of Limerick  Limerick V94 T9PX Republic of 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Number(s) 2105435 (forSOFOUR-1-Zn) and 2069812 (forSIFSIX-22-Zn)contain the supplementary crystallographic data for this paper. 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