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Although copper\u2010based catalysts have attracted much attention due to their low cost and high FOR activity, the performance enhancement mechanism lacks in\u2010depth investigation. Here, an amorphous\u2010crystalline catalyst of amorphous nickel hydroxide\u2010coated copper dendrites on copper foam (Cu@Ni(OH)\n                    <jats:sub>2<\/jats:sub>\n                    \/CF) is prepared. The modification of Ni(OH)\n                    <jats:sub>2<\/jats:sub>\n                    resulted in hydrophilic and aerophobic states on the Cu@Ni(OH)\n                    <jats:sub>2<\/jats:sub>\n                    \/CF surface, facilitating the transport of liquid\u2010phase species on the electrode surface and accelerating the release of H\n                    <jats:sub>2<\/jats:sub>\n                    . The Open circuit potential (OCP) and density functional theory (DFT) calculations indicate that this core\u2013shell structure facilitates the adsorption of HCHO and OH\n                    <jats:sup>\u2212<\/jats:sup>\n                    . In addition, the catalytic mechanism and reaction pathway of FOR are investigated through in situ FTIR and DFT calculations, and the results showed that the modification of Ni(OH)\n                    <jats:sub>2<\/jats:sub>\n                    lowered the energy barrier for C\u2500H bond breaking and H\u2500H bond formation. In the HER\/\/FOR system, Pt\/C\/\/Cu@Ni(OH)\n                    <jats:sub>2<\/jats:sub>\n                    \/CF can provide a current density of 0.5 A cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    at 0.36\u00a0V and achieve efficient and stable H\n                    <jats:sub>2<\/jats:sub>\n                    production. This work offers new ideas for designing electrocatalysts for bipolar hydrogen production system assisted with formaldehyde oxidation.\n                  <\/jats:p>","DOI":"10.1002\/smll.202410478","type":"journal-article","created":{"date-parts":[[2025,1,14]],"date-time":"2025-01-14T01:52:52Z","timestamp":1736819572000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":14,"title":["Amorphous Ni(OH)\n                    <sub>2<\/sub>\n                    Coated Cu Dendrites with Superaerophobic Interface for Bipolar Hydrogen Production Assisted with Formaldehyde Oxidation"],"prefix":"10.1002","volume":"21","author":[{"given":"Shaojian","family":"Jiang","sequence":"first","affiliation":[{"name":"State Key Laboratory Breeding Base of Green\u2010Chemical Synthesis Technology College of Chemical Engineering Zhejiang University of Technology  Hangzhou 310014 P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenke","family":"Liu","sequence":"additional","affiliation":[{"name":"State Key Laboratory Breeding Base of Green\u2010Chemical Synthesis Technology College of Chemical Engineering Zhejiang University of Technology  Hangzhou 310014 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kai","family":"Deng","sequence":"additional","affiliation":[{"name":"State Key Laboratory Breeding Base of Green\u2010Chemical Synthesis Technology College of Chemical Engineering Zhejiang University of Technology  Hangzhou 310014 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hongjie","family":"Yu","sequence":"additional","affiliation":[{"name":"State Key Laboratory Breeding Base of Green\u2010Chemical Synthesis Technology College of Chemical Engineering Zhejiang University of Technology  Hangzhou 310014 P. R. 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