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Here, we report NiMn\u2010based layered double hydroxide electrocatalysts (NiMn\u2010LDH) that enhance phenol degradation under mild electrochemical conditions. Mn incorporation into the LDH structure provides accessible higher oxidation states, improving redox flexibility, promoting hydroxyl radical (\u00b7OH) generation, and suppressing the competing oxygen evolution reaction. Three variants, NiMn\u2010LDH\u2010CNT, NiMn\u2010LDH\u2010CMC, and NiMn\u2010LDH\u2010Tris, were synthesized to assess the influence of conductive additives and synthesis media. The CNT\u2010supported catalyst showed the highest activity, achieving &gt;95% phenol removal within minutes at current densities up to 20\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , while maintaining a nearly constant cell voltage over approximately 200\u00a0h of operation. High removal efficiencies, ca. 90%, were retained even when the Na\n                    <jats:sub>2<\/jats:sub>\n                    SO\n                    <jats:sub>4<\/jats:sub>\n                    concentration was decreased from 100 to 1\u00a0mM and under synthetic wastewater conditions, confirming system robustness. The optimized NiMn\u2010LDH electrocatalyst was further integrated as the anode in a hybrid cell coupling phenol oxidation with CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction at a Cu\/CuO cathode, enabling simultaneous wastewater remediation and CO\n                    <jats:sub>2<\/jats:sub>\n                    conversion to value\u2010added hydrocarbons.\n                  <\/jats:p>","DOI":"10.1002\/gch2.70155","type":"journal-article","created":{"date-parts":[[2026,9,25]],"date-time":"2026-09-25T07:50:35Z","timestamp":1790322635000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Hybrid NiMn\u2010LDHs as Active Materials for Electro\u2010Oxidation of Organic Pollutants"],"prefix":"10.1002","volume":"10","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-3929-5497","authenticated-orcid":false,"given":"Keyvan","family":"Mirehbar","sequence":"first","affiliation":[{"name":"Electrochemical Processes Unit IMDEA Energy Institute  M\u00f3stoles, Madrid Spain"},{"name":"Escuela de Doctorado UAM, Centro de Estudios de Posgrado Universidad Aut\u00f3noma de Madrid, Ciudad Universitaria de Cantoblanco  Madrid Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Javier","family":"Llorente\u2010L\u00f3pez","sequence":"additional","affiliation":[{"name":"Photoactivated Processes Unit IMDEA Energy Institute  M\u00f3stoles, Madrid Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Alvaro","family":"Seijas\u2010Da Silva","sequence":"additional","affiliation":[{"name":"Institute of Molecular Science (ICMol) University of Valencia (UVEG)  Paterna Spain"},{"name":"Matteco Team, S.L., Carrer de Les Noves Tecnologies  Paterna, Valencia Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8163-5056","authenticated-orcid":false,"given":"Camilo","family":"Jaramillo\u2010Hern\u00e1ndez","sequence":"additional","affiliation":[{"name":"Institute of Molecular Science (ICMol) University of Valencia (UVEG)  Paterna Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-1218-9719","authenticated-orcid":false,"given":"Petra","family":"Batini\u0107","sequence":"additional","affiliation":[{"name":"Electrochemical Processes Unit IMDEA Energy Institute  M\u00f3stoles, Madrid Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Paula","family":"Porawski","sequence":"additional","affiliation":[{"name":"Electrochemical Processes Unit IMDEA Energy Institute  M\u00f3stoles, Madrid 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