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A promising and potentially greener alternative is electrochemical ammonia synthesis, though effective systems in this context are largely lacking. To this end, this study develops a reactor platform that integrates a palladium membrane reactor as a hydrogen conduit coupled with a mono\u2010terpyridine nickel molecular catalyst. This system achieved a peak Faradaic efficiency of 36% for ammonia production at a current density of \u22120.85\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    in a decoupled electrocatalytic manner. In situ spectroscopic analysis, electroanalytical techniques, and computational modelling have revealed a unique catalyst mechanism that entails the formation of a Ni\u2010H species generated from the active hydrogen from the Pd membrane as a key intermediate in the reaction route. The insights gained from this unique system stand to aid the development of practical ammonia production systems while expanding the community's knowledge base on dinitrogen activation.\n                  <\/jats:p>","DOI":"10.1002\/advs.78155","type":"journal-article","created":{"date-parts":[[2026,10,7]],"date-time":"2026-10-07T05:17:14Z","timestamp":1791350234000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Molecular Electrocatalysis Coupled With a Palladium Membrane Reactor Affords Selective Nitrogen Reduction"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-8636-5638","authenticated-orcid":false,"given":"Morgan","family":"McKee","sequence":"first","affiliation":[{"name":"Institute of Inorganic Chemistry University of Bonn  Bonn Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6391-8092","authenticated-orcid":false,"given":"Sai Phani Kumar","family":"Vangala","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering McGill University  Montr\u00e9al Qu\u00e9bec Canada"},{"name":"Department of Chemical Engineering Indian Institute of Science Education and Research (IISER) Bhopal  Bhopal Madhya Pradesh India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Farzaneh","family":"Farzinpour","sequence":"additional","affiliation":[{"name":"Institute of Inorganic Chemistry University of Bonn  Bonn Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-0435-3661","authenticated-orcid":false,"given":"Jasmin","family":"Wagner","sequence":"additional","affiliation":[{"name":"Institute of Inorganic Chemistry University of Bonn  Bonn Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-8220-8234","authenticated-orcid":false,"given":"Giacomo","family":"Pugliese","sequence":"additional","affiliation":[{"name":"Institute of Inorganic Chemistry University of Bonn  Bonn Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6804-1114","authenticated-orcid":false,"given":"Hamed","family":"Heidarpour","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering McGill University  Montr\u00e9al Qu\u00e9bec Canada"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7109-1910","authenticated-orcid":false,"given":"Hossein","family":"Bemana","sequence":"additional","affiliation":[{"name":"Institute of Inorganic Chemistry University of Bonn  Bonn Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7902-3066","authenticated-orcid":false,"given":"J. 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