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Conventional sequential treatments for their simultaneous removal face major issues of catalyst deactivation and byproduct generation. Here, we develop a subtle strategy using light\u2010induced ligand\u2010to\u2010metal charge transfer (LMCT) catalysis with Fe(II) ethylenediaminetetraacetic acid (EDTA\u2010Fe\u1d35\u1d35) to achieve redox\u2010coupled conversion of NO and SO\n                    <jats:sub>2<\/jats:sub>\n                    mixtures. LMCT excitation in EDTA\u2010Fe\n                    <jats:sup>II<\/jats:sup>\n                    induces directional charge separation under irradiation, routing photogenerated electrons (e\u207b) to Fe\u1d35\u1d35 for driving selective NO\u2010to\u2010N\n                    <jats:sub>2<\/jats:sub>\n                    conversion (selectivity: 99.89%), while photogenerated holes (h\n                    <jats:sup>+<\/jats:sup>\n                    ) oxidize SO\n                    <jats:sub>2<\/jats:sub>\n                    to SO\n                    <jats:sub>4<\/jats:sub>\n                    <jats:sup>2<\/jats:sup>\n                    \u207b (selectivity: 96.34%). This spatial segregation of redox pathways suppresses N\n                    <jats:sub>2<\/jats:sub>\n                    O generation, enabling continuous operation with 90.3% NO and nearly 100% SO\n                    <jats:sub>2<\/jats:sub>\n                    removal efficiency. Mechanism studies reveal the LMCT\u2010enhanced charge transfer from carboxyl\/amino groups to Fe centers, while in situ EPR confirms the \u2022SO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>2<\/jats:sup>\n                    \u207b radical\u2010mediated h\n                    <jats:sup>+<\/jats:sup>\n                    scavenging that accelerates charge separation and utilization. This work establishes Fe\u2010LMCT catalysis as a sustainable platform for gas\u2010phase pollutants remediation, achieving unprecedented selectivity through precise redox pathway control.\n                  <\/jats:p>","DOI":"10.1002\/anie.202510456","type":"journal-article","created":{"date-parts":[[2025,7,8]],"date-time":"2025-07-08T10:24:48Z","timestamp":1751970288000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["Light\u2010Induced Fe\u2010LMCT Catalysis for Redox\u2010Coupled Conversion of NO\n                    <sub>x<\/sub>\n                    and SO\n                    <sub>2<\/sub>\n                    Mixture"],"prefix":"10.1002","volume":"64","author":[{"given":"Ruimin","family":"Chen","sequence":"first","affiliation":[{"name":"Research Center for Carbon\u2010Neutral Environmental &amp; Energy Technology, Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China  Chengdu 611731 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jielin","family":"Wang","sequence":"additional","affiliation":[{"name":"Research Center for Carbon\u2010Neutral Environmental &amp; Energy Technology, Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China  Chengdu 611731 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Taobo","family":"Huang","sequence":"additional","affiliation":[{"name":"Department of Environmental Science and Engineering Fudan University  Shanghai 200433 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chunling","family":"Zhang","sequence":"additional","affiliation":[{"name":"Research Center for Carbon\u2010Neutral Environmental &amp; Energy Technology, Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China  Chengdu 611731 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiuping","family":"Zhu","sequence":"additional","affiliation":[{"name":"Department of Environmental Science and Engineering Fudan University  Shanghai 200433 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jieyuan","family":"Li","sequence":"additional","affiliation":[{"name":"Research Center for Carbon\u2010Neutral Environmental &amp; Energy Technology, Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China  Chengdu 611731 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2890-9964","authenticated-orcid":false,"given":"Fan","family":"Dong","sequence":"additional","affiliation":[{"name":"Research Center for Carbon\u2010Neutral Environmental &amp; Energy Technology, Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China  Chengdu 611731 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,7,14]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1038\/nature13774"},{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.est.1c06068"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.est.4c02997"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1021\/ie020709"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jenvman.2016.09.042"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2016.06.071"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.psep.2009.06.002"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.envres.2021.112541"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.energyfuels.8b03820"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1021\/es061757e"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2024.148583"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1021\/ie00097a002"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.est.8b03934"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.adq0302"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-020-2780-0"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41558-019-0613-7"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1002\/cctc.202200916"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.watres.2019.115375"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-024-50507-6"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-022-35344-9"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jphotochem.2006.11.030"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.est.2c09669"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.fuel.2023.129128"},{"key":"e_1_2_8_24_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jhazmat.2006.08.021"},{"key":"e_1_2_8_25_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2006.12.030"},{"key":"e_1_2_8_26_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.psep.2022.01.080"},{"key":"e_1_2_8_27_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.energyfuels.9b02984"},{"key":"e_1_2_8_28_1","doi-asserted-by":"publisher","DOI":"10.1002\/cphc.200900268"},{"key":"e_1_2_8_29_1","doi-asserted-by":"publisher","DOI":"10.1021\/ct2009363"},{"key":"e_1_2_8_30_1","first-page":"1007","volume":"90","author":"Dunning T. 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