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In this study, we presented an experimental realization of surface coverage modulation on a photoelectrode using a photo\u2010induced charge activation method. Through the surface coverage modulation, both pre\u2010oxidized alcohol substrates and surface coverage were increased, which not only improved the reaction kinetics but also suppressed the over\u2010oxidation of the generated aldehydes\/ketones. As a demonstration, the Faradaic efficiency for the conversion of glycerol to dihydroxyacetone increased from 31.8\u2009% to 46.8\u2009% (with selectivity rising from 47.6\u2009% to 71.3\u2009%), from 73.4\u2009% to 87.8\u2009% for benzyl alcohol to benzyl aldehyde (selectivity increasing from 76.7\u2009% to 92.4\u2009%) and from 4.2\u2009% to 53.6\u2009% for ethylene glycol to glycolaldehyde (selectivity increasing from 6.2\u2009% to 62.7\u2009%). Our findings offer a promising strategy for the production of high\u2010value carbon products in heterogeneous catalysis.<\/jats:p>","DOI":"10.1002\/anie.202423730","type":"journal-article","created":{"date-parts":[[2024,12,31]],"date-time":"2024-12-31T04:29:31Z","timestamp":1735619371000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Surface Coverage Tuning for Suppressing Over\u2010Oxidation: A Case of Photoelectrochemical Alcohol\u2010to\u2010Aldehyde\/Ketone Conversion"],"prefix":"10.1002","volume":"64","author":[{"given":"Chaoran","family":"Dong","sequence":"first","affiliation":[{"name":"Key Laboratory of Environmental Remediation and Ecological Health Ministry of Industry and Information Technology School of Environmental and Biological Engineering Nanjing University of Science and Technology  Nanjing 210094 China"},{"name":"School of Materials Science and Engineering Nanjing University of Science and Technology  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cheng","family":"Lin","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Nanjing University of Science and Technology  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Panjie","family":"Li","sequence":"additional","affiliation":[{"name":"Key Laboratory of Environmental Remediation and Ecological Health Ministry of Industry and Information Technology School of Environmental and Biological Engineering Nanjing University of Science and Technology  Nanjing 210094 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jong Hyeok","family":"Park","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering Yonsei University  50 Yonsei-ro, Seodaemun-gu Seoul, Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinyou","family":"Shen","sequence":"additional","affiliation":[{"name":"Key Laboratory of Environmental Remediation and Ecological Health Ministry of Industry and Information Technology School of Environmental and Biological Engineering Nanjing University of Science and Technology  Nanjing 210094 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1121-3426","authenticated-orcid":false,"given":"Kan","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Nanjing University of Science and Technology  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,1,9]]},"reference":[{"key":"e_1_2_7_1_1","unstructured":"\u00a0"},{"key":"e_1_2_7_2_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.6b00510"},{"key":"e_1_2_7_3_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201410738"},{"key":"e_1_2_7_4_1","unstructured":"\u00a0"},{"key":"e_1_2_7_5_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41570-024-00589-z"},{"key":"e_1_2_7_6_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.2c00602"},{"key":"e_1_2_7_7_2","doi-asserted-by":"publisher","DOI":"10.1038\/s44160-024-00499-4"},{"key":"e_1_2_7_8_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202209014"},{"key":"e_1_2_7_9_1","unstructured":"\u00a0"},{"key":"e_1_2_7_10_2","doi-asserted-by":"publisher","DOI":"10.1021\/ar010075n"},{"key":"e_1_2_7_11_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202009811"},{"key":"e_1_2_7_12_1","unstructured":"\u00a0"},{"key":"e_1_2_7_13_2","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202306488"},{"key":"e_1_2_7_14_2","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202304133"},{"key":"e_1_2_7_15_1","unstructured":"\u00a0"},{"key":"e_1_2_7_16_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.1195055"},{"key":"e_1_2_7_17_2","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.2c11117"},{"key":"e_1_2_7_18_2","volume":"60","author":"Zhao S.","year":"2021","journal-title":"Angew. 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