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To address these challenges, we strategically manage the generation and utilization of active hydrogen (H\n                    <jats:sup>*<\/jats:sup>\n                    ) by integrating metallic Cu with atomically dispersed Zn\u2212N\n                    <jats:sub>4<\/jats:sub>\n                    sites, thereby selectively increasing NH\n                    <jats:sub>3<\/jats:sub>\n                    production. In situ x\u2010ray absorption spectroscopy, in situ infrared, in situ Raman, and combined with theoretical calculations, systematically demonstrate that Zn\u2212N\n                    <jats:sub>4<\/jats:sub>\n                    sites facilitate water dissociation to generate and capture H\n                    <jats:sup>*<\/jats:sup>\n                    species. These H\n                    <jats:sup>*<\/jats:sup>\n                    species subsequently spill over to neighboring metallic Cu, which play a crucial role in NO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    adsorption and activation. The spatial separation effect between H\n                    <jats:sup>*<\/jats:sup>\n                    capture and utilization sites ensures continuous H\n                    <jats:sup>*<\/jats:sup>\n                    generation and supply, thus enhancing N\u2500H bond coupling for efficient NH\n                    <jats:sub>3<\/jats:sub>\n                    synthesis. As a result, the catalyst achieves a maximum NH\n                    <jats:sub>3<\/jats:sub>\n                    yield rate of 21.96\u00a0mg h\n                    <jats:sup>\u22121<\/jats:sup>\n                    cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    and a highest Faradaic efficiency (FE) of 97.07% in 0.1\u00a0M KNO\n                    <jats:sub>3<\/jats:sub>\n                    under alkaline media. The constructed Zn\u2010NO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    battery can deliver an impressive power density of 14.59\u00a0mW cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , a NH\n                    <jats:sub>3<\/jats:sub>\n                    yield rate of 4.26\u00a0mg h\n                    <jats:sup>\u22121<\/jats:sup>\n                    cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , and a FE of 93.65%, while consistently operating for over 100\u00a0h.\n                  <\/jats:p>","DOI":"10.1002\/anie.5589616","type":"journal-article","created":{"date-parts":[[2026,8,22]],"date-time":"2026-08-22T09:17:30Z","timestamp":1787390250000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Highly Selective Electrocatalytic Ammonia Synthesis Enabled by Spatial Separation of Active Hydrogen Capture and Spillover Sites"],"prefix":"10.1002","author":[{"given":"Qian","family":"Guo","sequence":"first","affiliation":[{"name":"Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People's Republic of China Heilongjiang University  Harbin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tianyu","family":"Han","sequence":"additional","affiliation":[{"name":"Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People's Republic of China Heilongjiang University  Harbin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yingsheng","family":"Zheng","sequence":"additional","affiliation":[{"name":"Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People's Republic of China Heilongjiang University  Harbin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0624-5098","authenticated-orcid":false,"given":"Lei","family":"Wang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People's Republic of China Heilongjiang University  Harbin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5800-451X","authenticated-orcid":false,"given":"Honggang","family":"Fu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People's Republic of China Heilongjiang University  Harbin China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,8,22]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560\u2010024\u201001622\u20107"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586\u2010022\u201005108\u2010y"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.abg2371"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202515346"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202202556"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1002\/ange.202320027"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.5c04411"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.est.3c09759"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/ange.202218717"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202500371"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.9b00202"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202415632"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2020.12.025"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202304021"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1002\/ange.202517259"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202505937"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929\u2010019\u20100280\u20100"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202423612"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2022.121805"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cjsc.2024.100447"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929\u2010018\u20100146\u2010x"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2022.139533"},{"key":"e_1_2_8_24_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202007345"},{"key":"e_1_2_8_25_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.nanoen.2019.02.055"},{"key":"e_1_2_8_26_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202422585"},{"key":"e_1_2_8_27_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202211098"},{"key":"e_1_2_8_28_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202500065"},{"key":"e_1_2_8_29_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsnano.5c08871"},{"key":"e_1_2_8_30_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202102053"},{"key":"e_1_2_8_31_1","doi-asserted-by":"publisher","DOI":"10.1002\/ange.202218717"},{"key":"e_1_2_8_32_1","doi-asserted-by":"publisher","DOI":"10.3390\/cryst8050225"},{"key":"e_1_2_8_33_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202600025"},{"key":"e_1_2_8_34_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.mattod.2025.02.012"},{"key":"e_1_2_8_35_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202509090"},{"key":"e_1_2_8_36_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.6c01046"},{"key":"e_1_2_8_37_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202514840"},{"key":"e_1_2_8_38_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202408758"},{"key":"e_1_2_8_39_1","doi-asserted-by":"publisher","DOI":"10.1002\/ange.7719126"},{"key":"e_1_2_8_40_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c16080"},{"key":"e_1_2_8_41_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010026\u201069802\u20105"},{"key":"e_1_2_8_42_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202501527"},{"key":"e_1_2_8_43_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202425262"},{"key":"e_1_2_8_44_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202502073"},{"key":"e_1_2_8_45_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c10516"},{"key":"e_1_2_8_46_1","doi-asserted-by":"publisher","DOI":"10.1039\/D2EE04095F"},{"key":"e_1_2_8_47_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202408382"},{"key":"e_1_2_8_48_1","doi-asserted-by":"publisher","DOI":"10.1002\/ange.202410356"},{"key":"e_1_2_8_49_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c06904"},{"key":"e_1_2_8_50_1","doi-asserted-by":"publisher","DOI":"10.1039\/D4EE00715H"},{"key":"e_1_2_8_51_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202409799"},{"key":"e_1_2_8_52_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010022\u201028728\u20104"},{"key":"e_1_2_8_53_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010024\u201048035\u20104"}],"container-title":["Angewandte 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