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Here we report an atomic\u2010level hydrogen pump that directionally regulates hydrogen flux across a well\u2010defined Cu\n                    <jats:sub>2<\/jats:sub>\n                    O@Co\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    core\u2013shell interface. By anchoring Pd single atoms either at the interface (Pd\u2010in) or on the outer shell (Pd\u2010out), we demonstrate that only the interfacial configuration enables efficient *H relay from Co\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    hydrogen\u2010generation sites to Cu\n                    <jats:sub>2<\/jats:sub>\n                    O nitrate\u2010reduction centers. This design suppresses *NO\n                    <jats:sub>2<\/jats:sub>\n                    accumulation and minimizes hydrogen evolution, achieving a near\u2010unity Faradaic efficiency of 99.9% and an exceptional NH\n                    <jats:sub>3<\/jats:sub>\n                    yield of 63.9\u00a0mg h\n                    <jats:sup>\u22121<\/jats:sup>\n                    mg\n                    <jats:sub>cat<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    at \u22120.55\u00a0V versus RHE, outperforming most reported systems. Operando spectroscopy, kinetic isotope effects (KIEs), and DFT calculations reveal that interfacial Pd lowers the *H migration barrier from 1.21 to 1.01\u00a0eV, thereby kinetically favoring hydrogenation over HER. The generality of this hydrogen\u2010pump mechanism is further demonstrated in urea synthesis, hydrodehalogenation of 2,4,6\u2010tribromophenol, and Zn\u2010NO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    battery systems. These findings establish hydrogen flux regulation via single\u2010atom positioning as a general strategy for optimizing multi\u2010step electrocatalytic reactions.\n                  <\/jats:p>","DOI":"10.1002\/adma.75022","type":"journal-article","created":{"date-parts":[[2026,9,15]],"date-time":"2026-09-15T10:21:44Z","timestamp":1789467704000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Atomic\u2010Level Hydrogen Pumping Enables Near\u2010Unity Faradaic Efficiency in Nitrate\u2010to\u2010Ammonia Electroreduction"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-9493-3468","authenticated-orcid":false,"given":"Tianbo","family":"Jia","sequence":"first","affiliation":[{"name":"State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences  Taiyuan China"},{"name":"School of Petrochemical Engineering &amp; Environment Zhejiang Ocean University  Zhoushan China"},{"name":"University of Chinese Academy of Sciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lei","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences  Taiyuan China"},{"name":"University of Chinese Academy of Sciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuying","family":"Gao","sequence":"additional","affiliation":[{"name":"School of Petrochemical Engineering &amp; Environment Zhejiang Ocean University  Zhoushan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8481-3225","authenticated-orcid":false,"given":"Yuchuan","family":"Ye","sequence":"additional","affiliation":[{"name":"School of Petrochemical Engineering &amp; Environment Zhejiang Ocean University  Zhoushan China"},{"name":"Ocean College Zhejiang University  Zhoushan 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Zhejiang Ocean University  Zhoushan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinshu","family":"Lu","sequence":"additional","affiliation":[{"name":"School of Petrochemical Engineering &amp; Environment Zhejiang Ocean University  Zhoushan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9007-4817","authenticated-orcid":false,"given":"Min","family":"Liu","sequence":"additional","affiliation":[{"name":"Hunan Joint International Research Center for Carbon Dioxide Resource Utilization State Key Laboratory of Powder Metallurgy School of Physics and Electronics Central South University  Changsha China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9308-6074","authenticated-orcid":false,"given":"Chaoqiu","family":"Chen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences  Taiyuan China"},{"name":"University of Chinese Academy of Sciences  Beijing China"},{"name":"Shanxi Key Laboratory for the Green Catalysis Synthesis of Coal\u2010based Value\u2010Added Chemicals Shanxi University  Taiyuan China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,9,15]]},"reference":[{"key":"e_1_2_9_2_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202422585"},{"key":"e_1_2_9_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202315324"},{"key":"e_1_2_9_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202521409"},{"key":"e_1_2_9_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202308775"},{"key":"e_1_2_9_6_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202004523"},{"key":"e_1_2_9_7_1","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.2306461120"},{"key":"e_1_2_9_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpclett.5c00563"},{"key":"e_1_2_9_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202404194"},{"key":"e_1_2_9_10_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010025\u201060043\u20106"},{"key":"e_1_2_9_11_1","doi-asserted-by":"publisher","DOI":"10.1007\/s40820\u2010023\u201001217\u2010z"},{"key":"e_1_2_9_12_1","doi-asserted-by":"publisher","DOI":"10.1039\/D1EE03097C"},{"key":"e_1_2_9_13_1","doi-asserted-by":"crossref","DOI":"10.1002\/anie.202420903","article-title":"Selenium\u2010Deficient 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Augmented\u2010Wave Method","volume":"50","author":"Bl\u00f6chl P. 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