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However, this process is often hampered by the low efficiency of C\n                    <jats:sub>5+<\/jats:sub>\n                    alcohol (C\n                    <jats:sub>5+<\/jats:sub>\n                    OH) synthesis, high catalyst production costs, and limited water tolerance. Here, we report for the first time a low\u2010cost, high\u2010performance Ni\u2010based catalyst synthesized via a precise surface selenization protocol that effectively overcomes these limitations. The optimized catalyst significantly outperforms noble metal catalysts, achieving a total alcohol yield of 62.6% and a high selectivity of 83.8% for HAS (62.0% for C\n                    <jats:sub>5+<\/jats:sub>\n                    OH) in the cross\u2010condensation of MeOH and EtOH. Our characterizations and theoretical simulations indicate that Se doping restructures the Ni surface, creating three\u2010coordinated Ni\u2500Se sites. These sites promote efficient alcohol dehydrogenation and raise the energy barrier for aldehyde decomposition, thereby greatly increasing the efficiency and selectivity of MeOH and EtOH cross\u2010condensation to C\n                    <jats:sub>5+<\/jats:sub>\n                    OH.\n                  <\/jats:p>","DOI":"10.1002\/anie.202510601","type":"journal-article","created":{"date-parts":[[2025,7,18]],"date-time":"2025-07-18T06:48:23Z","timestamp":1752821303000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Restructured Three\u2010Coordinated Ni\u2500Se Catalytic Sites for Enhanced Cross\u2010Condensation of Methanol and Ethanol"],"prefix":"10.1002","volume":"64","author":[{"given":"Juwen","family":"Gu","sequence":"first","affiliation":[{"name":"School of Chemical Engineering and Light Industry Guangdong University of Technology  Guangzhou 510006 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Microscale University of Science and Technology of China  Hefei 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiawei","family":"Li","sequence":"additional","affiliation":[{"name":"School of Nuclear Science and Technology Key Laboratory of Precision and Intelligent Chemistry National Synchrotron Radiation Laboratory School of Chemistry and Materials Science Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China  Hefei 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Songbai","family":"Qiu","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Light Industry Guangdong University of Technology  Guangzhou 510006 China"},{"name":"Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center  Jieyang 515200 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tiejun","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Light Industry Guangdong University of Technology  Guangzhou 510006 China"},{"name":"Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center  Jieyang 515200 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tian","family":"Sheng","sequence":"additional","affiliation":[{"name":"Key Laboratory of Functional Molecular Solids Ministry of Education Anhui Key Laboratory of Molecule\u2010Based Materials Anhui Engineering Research Center of Carbon Neutrality College of Chemistry and Materials Science Anhui Normal University  Wuhu 241002 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1995-8257","authenticated-orcid":false,"given":"Yujie","family":"Xiong","sequence":"additional","affiliation":[{"name":"School of Nuclear Science and Technology Key Laboratory of Precision and Intelligent Chemistry National Synchrotron Radiation Laboratory School of Chemistry and Materials Science Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China  Hefei 230026 China"},{"name":"Key Laboratory of Functional Molecular Solids Ministry of Education Anhui Key Laboratory of Molecule\u2010Based Materials Anhui Engineering Research Center of Carbon Neutrality College of Chemistry and Materials Science Anhui Normal University  Wuhu 241002 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,7,17]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1016\/S0306-2619(02)00184-8"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.rser.2017.05.063"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-024-46513-3"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202207278"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202210991"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202406761"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-018-07593-0"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202008289"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1039\/D0EE01860K"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-018-03543-y"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.1c04626"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1038\/nature06450"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1039\/C5GC02963E"},{"key":"e_1_2_7_14_1","doi-asserted-by":"publisher","DOI":"10.1002\/cssc.201801690"},{"key":"e_1_2_7_15_1","doi-asserted-by":"publisher","DOI":"10.1039\/C5CY00359H"},{"key":"e_1_2_7_16_1","first-page":"19","volume-title":"Ullmann's 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