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A new method, the Ce\u2010enhanced modulation of MOFs\u2019 microenvironment, is proposed to modulate the \u2013COO\u00b7\u00b7\u00b7Cu(II)\u2013 coordination microenvironment of Hong Kong University of Science and Technology (HKUST\u20101) using Ce(III) as a molecular scalpel for fabricating abundant high\u2010efficiency Cu(I) and Cu\u2010coordination\u2010unsaturated sites and improving the pore structures around adsorptive sites. The optimal CH\u2010250 thus exhibits adsorptive capacities for 20.2, 28.0, and 58.3\u00a0mg\u00a0S\u00a0g<jats:sup>\u20131<\/jats:sup> of thiophene, benzo\u2010thiophene, and dibenzothiophene, respectively, which are superior to most reported MOFs, zeolites, and nanoporous carbons. The constructed Cu(I) sites show stronger affinity for dibenzothiophene (\u22120.86\u00a0eV) than the initial Cu(II) (\u22120.74\u00a0eV) for out\u2010of\u2010plane adsorption. Further, they are far stronger in\u2010plane adsorption interactions in DBT\/CH\u2010250 (\u22120.90\u00a0eV) than those in DBT\/HKUST\u20101 (\u22120.37\u00a0eV). Thus, molecular engineering for modulating the coordination microenvironment of MOFs shows great potential for adsorption desulfurization.<\/jats:p>","DOI":"10.1002\/smll.202304644","type":"journal-article","created":{"date-parts":[[2023,8,11]],"date-time":"2023-08-11T05:13:55Z","timestamp":1691730835000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":14,"title":["Enhancing Adsorption Desulfurization Performance Using Enriched Cu(I) Sites over Microenvironment\u2010Modulated HKUST\u20101"],"prefix":"10.1002","volume":"19","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-9031-9055","authenticated-orcid":false,"given":"Ping","family":"Lu","sequence":"first","affiliation":[{"name":"School of Chemical Engineering Fuzhou University  Fuzhou Fujian 350108 P. R. 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