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Here, we present a \u201ctwo\u2010in\u2010one\u201d photoreduction strategy enabled by electron\u2010rich Cd sites, both remote from and adjacent to sulfur vacancies (Vs). This strategy is highly selective for the reduction of O\n                    <jats:sub>2<\/jats:sub>\n                    and carbon dioxide radical anions (\u2022CO\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    ) in situ formed on the Bi\n                    <jats:sub>2<\/jats:sub>\n                    S\n                    <jats:sub>3<\/jats:sub>\n                    composition (hole) through water oxidation and oxalic acid (OA) oxidative C\u2013C cleavage, respectively. The shell\u2010yolk Z\u2010scheme Bi\n                    <jats:sub>2<\/jats:sub>\n                    S\n                    <jats:sub>3<\/jats:sub>\n                    \/CdS\u2010Vs achieves complete photothermal catalytic upgrading of OA to CO with an unprecedented yield (1671 \u00b5mol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) and selectivity &gt; 99%, outperforming state\u2010of\u2010the\u2010art photocatalysts for CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010to\u2010CO reduction. Mechanistic investigations reveal that shell Bi\n                    <jats:sub>2<\/jats:sub>\n                    S\n                    <jats:sub>3<\/jats:sub>\n                    can cooperate with \u2022OH generated\/transferred from the yolk CdS\u2010Vs to mediate the efficient production of \u2022CO\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>\u2012<\/jats:sup>\n                    . Hollow microenvironment and electronic structure of the yolk CdS\u2010Vs can be manipulated by Vs to increase enrichment of \u2022CO\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    and favor its proton\u2010coupled electron transfer to produce CO. Bi\n                    <jats:sub>2<\/jats:sub>\n                    S\n                    <jats:sub>3<\/jats:sub>\n                    \/CdS\u2010Vs exhibits good reusability and universality for converting various bio\u2010organic acids into CO with 94%\u2012100% selectivity. Tailor\u2010made versatile photocatalysts via vacancy engineering provide a viable avenue for the full\u2010carbon upcycling of biomass and waste sources to biofuels.\n                  <\/jats:p>","DOI":"10.1002\/anie.9066578","type":"journal-article","created":{"date-parts":[[2026,5,27]],"date-time":"2026-05-27T07:19:58Z","timestamp":1779866398000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Quantitative Photo\u2010Reforming of Biomass to CO Spurred by In Situ Protonation of Carbon Dioxide Radical Anions"],"prefix":"10.1002","volume":"65","author":[{"given":"Tengyu","family":"Liu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Green Pesticides State\u2010Local Joint Laboratory For Comprehensive Utilization of Biomass Center For R&amp;D of Fine Chemicals Guizhou University  Guiyang 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