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Here, we develop a computation\u2010guided strategy\u2014localized hydrogen\u2010affinity engineering\u2014to synthesize heteroatom\u2010decorated Cu hydrogenase for aldehydes electrification. Remarkably, the as\u2010prepared Rh\u2010decorated Cu hydrogenase (Rh\n                    <jats:sub>1<\/jats:sub>\n                    Cu\u2010Hase) achieves a remarkable Faraday efficiency of &gt;99.3% for formaldehyde conversion at an ultrahigh current density of 500 mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    with a minimal overpotential of 283 mV. A membrane\u2010free electrolyzer equipped with the Rh\n                    <jats:sub>1<\/jats:sub>\n                    Cu\u2010Hase operates stably for over 1200 h at 1000 mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , continuously producing high\u2010purity potassium diformate (KDF) and hydrogen. Techno\u2010economic analysis reveals a significant $166.1\/ton KDF revenue advantage over conventional methods. The paired dehydrogenation mechanism is proposed by a series of operando studies and theoretical calculations, unveiling that the Cu matrix facilitates aldehyde adsorption, while atomic Rh sites activate hydrogen, collectively reducing energy barriers for both C\u2500H cleavage and H\u2500H coupling. Furthermore, the universality of this strategy is demonstrated by its successful application in electrifying a broad range of industrially relevant aldehydes.\n                  <\/jats:p>","DOI":"10.1002\/anie.202515456","type":"journal-article","created":{"date-parts":[[2026,2,22]],"date-time":"2026-02-22T14:11:44Z","timestamp":1771769504000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":8,"title":["Industrial\u2010scale Aldehydes Electrification Via Localized Hydrogen\u2010affinity Engineering"],"prefix":"10.1002","volume":"65","author":[{"given":"Lei","family":"Shi","sequence":"first","affiliation":[{"name":"CAS Key Laboratory of Nanosystem and Hierarchical Fabrication National Center for Nanoscience and Technology  Beijing P.R. 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