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Direct selective hydrogenation of lignin derivatives has great potential for producing these chemicals, but is challenging to obtain high yields. Here, we report that hydrotalcite\u2010supported Pd single\u2010atom (Pd\/CHT\u2010800) catalyst enabled the hydrogenation of the benzene ring in the aromatics without the overreaction of carbonyl group, which could afford &gt;99.9% yield of cyclohexanones using water as the reaction medium. The reaction mechanism was systematically studied by the control experiments and detailed in situ characterizations. In the Pd\/CHT\u2010800 catalyst, the Pd\u2010O\u2010MgAl sites were formed, and the cooperation of the Pd atoms and calcined CHT material could not only realize the aromatic hydrogenation efficiently, but also inhibit the hydrogenation of the carbonyl group in the reaction effectively. This work provides a novel route for the sustainable production of cyclohexanones.<\/jats:p>","DOI":"10.1002\/anie.202504260","type":"journal-article","created":{"date-parts":[[2025,5,19]],"date-time":"2025-05-19T13:02:07Z","timestamp":1747659727000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":17,"title":["Selective Hydrogenation of Phenols to Cyclohexanones Over Hydrotalcite\u2010Supported Pd Single\u2010Atom Catalyst"],"prefix":"10.1002","volume":"64","author":[{"given":"Yani","family":"Liu","sequence":"first","affiliation":[{"name":"Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular &amp; Process Engineering School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 China"},{"name":"Institute of Eco\u2010Chongming 20 Cuiniao Road, Chenjia Town, Chongming District Shanghai 202162 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