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Here, we design Ag\/CoNiS heterostructures in which Ag loading density programs interfacial confinement to regulate hydrogen spillover from CoNiS water\u2010activation domains to Ag\u2010associated nitrate\/nitrogen oxide (NO\n                    <jats:sub>x<\/jats:sub>\n                    ) intermediates, thereby coupling\n                    <jats:sup>*<\/jats:sup>\n                    H generation, relay, and deep nitrate hydrogenation. The optimized Ag\n                    <jats:sub>M<\/jats:sub>\n                    \/CoNiS achieves an NH\n                    <jats:sub>3<\/jats:sub>\n                    yield of 22.31\u00a0mg\u00a0h\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    with 99.13% Faradaic efficiency. In situ Raman, distribution of relaxation times (DRT) analysis, hydrogen\/deuterium (H\/D) isotope experiments, and tert\u2010butanol (TBA) perturbation tests reveal that the confined Ag\u2013CoNiS interface regulates interfacial water and establishes a balanced\n                    <jats:sup>*<\/jats:sup>\n                    H supply\u2013consumption regime, thereby suppressing competing hydrogen evolution. Density functional theory (DFT) calculations further show that Ag facilitates nitrate deoxygenation, whereas excessive Ag coverage weakens Co\/Ni\u2010centered water activation, explaining the volcano\u2010type activity trend. Coupling NO\n                    <jats:sub>3<\/jats:sub>\n                    RR with the sulfide oxidation reaction (SOR) further enables a low\u2010voltage NO\n                    <jats:sub>3<\/jats:sub>\n                    RR||SOR electrolyzer, requiring only 0.70\u00a0V at 50\u00a0mA\u00a0cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    for energy\u2010saving co\u2010production of ammonia and sulfur.\n                  <\/jats:p>","DOI":"10.1002\/adma.73885","type":"journal-article","created":{"date-parts":[[2026,6,29]],"date-time":"2026-06-29T11:23:12Z","timestamp":1782732192000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Interfacial Confinement\u2010Programmed Hydrogen Spillover on Ag\/CoNiS Boosts Nitrate\u2010to\u2010Ammonia Electrosynthesis"],"prefix":"10.1002","volume":"38","author":[{"given":"Fengting","family":"Xie","sequence":"first","affiliation":[{"name":"State Key Laboratory of Advanced Fiber Materials College of Materials Science and Engineering Donghua University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xuxin","family":"Kang","sequence":"additional","affiliation":[{"name":"School of Physical Science and Technology Ningbo University  Ningbo China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zongtai","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of High\u2010Efficiency Flexible Coal Power Generation and Carbon Capture Utilization and Storage Xi'an Thermal Power Research Institute Co., Ltd.  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Honglin","family":"Zhu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Fiber Materials College of Materials Science and Engineering Donghua University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1931-7767","authenticated-orcid":false,"given":"Lei","family":"Wang","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering National University of Singapore  Singapore Singapore"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0779-2285","authenticated-orcid":false,"given":"Ziyang","family":"Wu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Fiber Materials College of Materials Science and Engineering Donghua University  Shanghai 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