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In particular, the electrocatalytic reductive amination (ERA) of 5\u2010hydroxymethylfurfural (5\u2010HMF) with ethanolamine provides a green alternative to conventional reductive amination by circumventing the use of high\u2010pressure H\n                    <jats:sub>2<\/jats:sub>\n                    and stoichiometric chemical reductants. Herein, we report a facet\u2010regulated CeO\n                    <jats:sub>2<\/jats:sub>\n                    catalyst that preferentially exposes vacancy\u2010derived frustrated Lewis pair (FLP) sites on the (100) surface, enabling highly efficient and selective ERA to produce 2\u2010[(5\u2010(hydroxymethyl)furan\u20102\u2010yl)methylamino]ethanol (HEMF). The optimized catalyst delivers 100% HEMF selectivity and a Faradaic efficiency of 99% at a current density of 20\u2009mA\u2009cm\n                    <jats:sup>\u20132<\/jats:sup>\n                    . Electrochemical measurements, high\u2010resolution transmission electron microscopy, temperature\u2010programmed desorption, and in situ ATR\u2010SEIRAS reveal that the vacancy\u2010derived FLP sites promote the cooperative adsorption of the imine intermediate and activation of its C\u2550N bond, thereby highlighting the decisive role of vacancy configuration in governing catalytic performance. These findings establish vacancy\u2010derived FLP sites as the key catalytic motifs for selective ERA and identify vacancy configuration engineering as an effective strategy for the rational design of highly efficient CeO\n                    <jats:sub>2<\/jats:sub>\n                    electrocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/cssc.71096","type":"journal-article","created":{"date-parts":[[2026,9,24]],"date-time":"2026-09-24T12:34:06Z","timestamp":1790253246000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Selective Electroreductive Amination of 5\u2010HMF Enabled by Facet\u2010Engineered Frustrated Lewis Pair\u2010Type Oxygen Vacancies on CeO\n                    <sub>2<\/sub>\n                    Nanocrystals"],"prefix":"10.1002","volume":"19","author":[{"given":"Yi\u2010Fei","family":"Zhang","sequence":"first","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences (BNLMS) State Key Laboratory of Rare Earth Materials Chemistry and Applications PKU\u2010HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry College of Chemistry and Molecular Engineering Peking University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiang","family":"Shao","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences (BNLMS) State Key Laboratory of Rare Earth Materials Chemistry and Applications PKU\u2010HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry College of Chemistry and Molecular Engineering Peking University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1007-1673","authenticated-orcid":false,"given":"Hao","family":"Dong","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences (BNLMS) State Key Laboratory of Rare Earth Materials Chemistry and 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