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In the state\u2010of\u2010the\u2010art, most of the studies on photocatalytic acetylene hydrogenation (PAH) were achieved by cobalt\u2010based photocatalysts, while the studies on the influence of microenvironment of cobalt catalytic active sites remain limited. Herein, via coordination ligand modulation method, we chose three 2D metal organic framework (2D MOFs) with different coordinated atoms (N, O, and S) around cobalt center and afforded CoN\n                    <jats:sub>4<\/jats:sub>\n                    MOF, CoO\n                    <jats:sub>4<\/jats:sub>\n                    MOF, and CoS\n                    <jats:sub>4<\/jats:sub>\n                    MOF, respectively, for studying the influence of coordination environment of cobalt active sites on photocatalytic C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    reduction. As a result, CoO\n                    <jats:sub>4<\/jats:sub>\n                    MOF with O\u2010coordinated cobalt sites exhibited the highest activity with C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    \u2010to\u2010C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    yield of 852.68\u00a0\u00b5mol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    in C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    atmosphere. Interestingly, in simulated industry\u2010relevant conditions gas with 1% C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    contained C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    mixture, CoN\n                    <jats:sub>4<\/jats:sub>\n                    MOF showed the optimal performance with near 100% conversion of low\u2010concentrated C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    . The photophysical, C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    adsorption characterization, in situ FTIR, and density functional theory (DFT) calculation were conducted to investigate the reaction mechanism. The results demonstrated that the O\u2010coordinated Co sites behaved more favorably thermodynamically for *C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    \u2010to\u2010*CH\n                    <jats:sub>2<\/jats:sub>\n                    CH intermediate, which caused superior activity. In contrast, the N\u2010coordinated Co sites showed highly efficient PAH in C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    rich conditions with low concentrated C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    due to the weak C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    competitive adsorption. This work is the first to explore the dependence of the active site coordination microenvironment for C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    photoreduction and provides a platform for constructing highly selective photocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.202522056","type":"journal-article","created":{"date-parts":[[2026,1,2]],"date-time":"2026-01-02T06:02:36Z","timestamp":1767333756000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["The Coordination Microenvironment Tailoring in 2D MOFs for Enhancing Photocatalytic Acetylene Semi\u2010Hydrogenation"],"prefix":"10.1002","volume":"65","author":[{"given":"Yu\u2010Fei","family":"Liu","sequence":"first","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou 510006 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ze\u2010Hui","family":"Li","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou 510006 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ming\u2010Yi","family":"Yang","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou 510006 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuai\u2010Bing","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Chemistry and Environment Engineering Changchun University of Science and Technology  Changchun 130022 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Han","family":"Zhang","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou 510006 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yong\u2010Jun","family":"Chen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Structural Chemistry Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences (CAS)  Fuzhou Fujian 350002 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mi","family":"Zhang","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou 510006 P.R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,1,1]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.1700782"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.3c00587"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202423091"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.iecr.9b04604"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929\u2010021\u201000640\u2010y"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2021.134129"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-021-26473-8"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aax8666"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aat0586"},{"key":"e_1_2_7_10_1","first-page":"1237","volume":"36","author":"Pang B. 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