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As such, pre\u2010installed active sites on catalysts are employed to mimic the natural secondary coordination environment for chemical transformations. Herein, we identify that varying the concentration of substrate (KNO\n                    <jats:sub>3<\/jats:sub>\n                    ), rather than pre\u2010installed motifs surrounding active sites of photocatalyst CdS quantum dots, forms a secondary coordination environment in situ. Spectroscopic and kinetic studies reveal that the in situ secondary coordination environment controls the reaction pathways and product selectivity of benzyl alcohol oxidation, synthetically valuable yet competitive pathways. Upon irradiation of photocatalyst CdS quantum dots, deoxybenzoin is obtained with 88.2% yield and 90.4\u00a0mmol\u00b7g\n                    <jats:sub>cat<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00b7h\n                    <jats:sup>\u22121<\/jats:sup>\n                    formation rate at 50\u00a0mM KNO\n                    <jats:sub>3<\/jats:sub>\n                    , while benzaldehyde is obtained with 87.2% yield and a formation rate of 357.4\u00a0mmol\u00b7g\n                    <jats:sub>cat<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00b7h\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 200\u00a0mM KNO\n                    <jats:sub>3<\/jats:sub>\n                    . Such a profound difference in product selectivity has not yet been realized. Different from pre\u2010installed active sites, simply varying substrate concentration in situ enables efficient regulation of reaction pathways and product selectivity of chemical transformation.\n                  <\/jats:p>","DOI":"10.1002\/anie.7505094","type":"journal-article","created":{"date-parts":[[2026,10,7]],"date-time":"2026-10-07T06:49:36Z","timestamp":1791355776000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Substrates In Situ Formed Dynamic Secondary Coordination Environment Regulates Reaction Pathways and Product Selectivity"],"prefix":"10.1002","author":[{"given":"Jia\u2010Hao","family":"Li","sequence":"first","affiliation":[{"name":"Key Laboratory of Supramolecular Photochemistry &amp; CAS\u2010HKU Joint Laboratory On New Materials, New Cornerstone Science Laboratory, Technical Institute of Physics and Chemistry Chinese Academy of Sciences  Beijing P. R. 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