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Herein, we first reported the discovery of acridine derivatives\n                    <jats:bold>(DADN<\/jats:bold>\n                    ,\n                    <jats:bold>PXZN<\/jats:bold>\n                    , and\n                    <jats:bold>PTZN<\/jats:bold>\n                    ) as new\u2010type, metal\u2010free, self\u2010sensitized molecule catalysts that enabled exceptional performance in solar\u2010driven CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction to formic acid. Notably, the atomically engineered sulfur\u2010containing heterocycle\n                    <jats:bold>PTZN<\/jats:bold>\n                    demonstrated unprecedented formate yield rate of 47.8\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    and &gt;99% selectivity in a photocatalytic system using 1,3\u2010dimethyl\u20101\n                    <jats:italic>H<\/jats:italic>\n                    \u2010benzo[\n                    <jats:italic>d<\/jats:italic>\n                    ]imidazol\u20103\u2010ium (BI\n                    <jats:sup>+<\/jats:sup>\n                    ) as proton and electron relay. The superior activity of\n                    <jats:bold>PTZN<\/jats:bold>\n                    was revealed to arise from its synergistic combination of strong CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010binding affinity (\u22120.195\u00a0eV), prolonged charge\u2010separated states (11\u00a0ns), and robust CO\n                    <jats:sub>2<\/jats:sub>\n                    electronic coupling (2.51\u00a0eV). Comprehensive studies including in situ electron spin resonance, in situ infrared, and transient absorption spectroscopy unambiguously unveiled a direct single electron transfer process from the excited singlet\u2010state acridine derivatives to CO\n                    <jats:sub>2<\/jats:sub>\n                    , generating CO\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>\u00b7\u2212<\/jats:sup>\n                    . Moreover, a hydrogen atom transfer process utilizing in situ generated BIH as a hydrogen atom carrier enabled the conversion of CO\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>\u00b7\u2212<\/jats:sup>\n                    to formic acid. This work establishes the first demonstration of a sequential proton\u2013electron transfer mechanism in acridine\u2010based photocatalysis, resolving long\u2010standing challenges in proton and electron delivery during CO\n                    <jats:sub>2<\/jats:sub>\n                    activation.\n                  <\/jats:p>","DOI":"10.1002\/anie.202508620","type":"journal-article","created":{"date-parts":[[2025,6,3]],"date-time":"2025-06-03T10:55:36Z","timestamp":1748948136000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":12,"title":["Atomically Engineered Acridine Derivatives Serve as Metal\u2010Free and Self\u2010Sensitized Catalysts for Solar\u2010Driven CO\n                    <sub>2<\/sub>\n                    to Formic Acid with High\u2010Efficiency and Near\u2010Perfect Selectivity"],"prefix":"10.1002","volume":"64","author":[{"given":"Xianjun","family":"Yin","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Mater Science and Engineering College of Chemistry Beijing University of Chemical Technology  Beijing 100084 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kefan","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Mater Science and Engineering College of Chemistry Beijing University of Chemical Technology  Beijing 100084 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cui","family":"Xu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Mater Science and Engineering College of Chemistry Beijing University of Chemical Technology  Beijing 100084 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Beijing 100190 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hui\u2010Qing","family":"Peng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Mater Science and Engineering College of Chemistry Beijing University of Chemical Technology  Beijing 100084 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chen\u2010Ho","family":"Tung","sequence":"additional","affiliation":[{"name":"Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences  Beijing 100190 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Li\u2010Zhu","family":"Wu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences  Beijing 100190 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