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In this work, efficient ethanol dehydrogenation was achieved at the anode of a high\u2010temperature polymer electrolyte membrane electrolyzer by integrating thermocatalytic ethanol dehydrogenation (EDHR) with electrochemical hydrogen oxidation (HOR) over Ru\/C and PdAu\/C composite catalytic layer. The Ru\/C serves as a bifunctional catalyst for the EDHR and HOR, and the PdAu\/C could rapidly electrooxidize retained acetaldehyde of the catalyst layer into acetic acid, thereby effectively promoting the dehydrogenation of ethanol. Under the conditions of 200 \u00b0C and 0.6\u00a0V, this reaction enabled high production rates of acetaldehyde (1479\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    with 99.06% selectivity) at the anode and H\n                    <jats:sub>2<\/jats:sub>\n                    (1728\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) at the cathode, substantially outperforming traditional thermal catalytic and electrocatalytic processes. This work provides a novel strategy for efficient alcohol dehydrogenation and facilitates the sustainable synthesis of value\u2010added products.\n                  <\/jats:p>","DOI":"10.1002\/anie.202525825","type":"journal-article","created":{"date-parts":[[2025,12,31]],"date-time":"2025-12-31T07:27:25Z","timestamp":1767166045000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Efficient Ethanol Dehydrogenation to Acetaldehyde and H\n                    <sub>2<\/sub>\n                    via Synergistic Thermocatalysis and Electrocatalysis"],"prefix":"10.1002","volume":"65","author":[{"given":"Jingjing","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Lab of Energy Electrochemistry of the Ministry of Education Hunan University  Changsha 410082 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Education Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qie","family":"Liu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Lab of Energy Electrochemistry of the Ministry of Education Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Miaoyu","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Lab of Energy Electrochemistry of the Ministry of Education Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Le","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Lab of Energy Electrochemistry of the Ministry of Education Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tehua","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Lab of Energy Electrochemistry of the Ministry of Education Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ru","family":"Chen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Lab of Energy Electrochemistry of the Ministry of Education Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhaoling","family":"Ma","sequence":"additional","affiliation":[{"name":"Guangxi Key Laboratory of Low Carbon Energy Materials Guangxi New Energy Ship Battery Engineering Technology Research Center Guangxi scientific and technological achievements transformation pilot research base of electrochemical energy materials and devices School of Chemistry and Pharmaceutical Sciences Guangxi Normal University  Guangxi 541004 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5206-1962","authenticated-orcid":false,"given":"Li","family":"Tao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Lab of Energy Electrochemistry of the Ministry of Education Hunan University  Changsha 410082 China"},{"name":"Greater Bay Area Institute for Innovation Hunan University  Guangzhou 511300 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuangyin","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Lab of Energy Electrochemistry of the Ministry of Education Hunan University  Changsha 410082 China"},{"name":"Greater Bay Area Institute for Innovation Hunan University  Guangzhou 511300 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