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Herein, we systematically synthesize a series of three V\/W mixed\u2010addenda polyoxometalate ([P\n                    <jats:sub>2<\/jats:sub>\n                    W\n                    <jats:sup>VI<\/jats:sup>\n                    <jats:sub>17<\/jats:sub>\n                    V\n                    <jats:sup>V<\/jats:sup>\n                    <jats:sub>1<\/jats:sub>\n                    O\n                    <jats:sub>62<\/jats:sub>\n                    ]\n                    <jats:sup>7\u2212<\/jats:sup>\n                    , noted as P\n                    <jats:sub>2<\/jats:sub>\n                    W\n                    <jats:sub>17<\/jats:sub>\n                    V\n                    <jats:sub>1<\/jats:sub>\n                    ) based metal\u2013organic frameworks [X\n                    <jats:sub>9<\/jats:sub>\n                    (DPYB)\n                    <jats:sub>9<\/jats:sub>\n                    (OX)\n                    <jats:sub>6<\/jats:sub>\n                    (H\n                    <jats:sub>2<\/jats:sub>\n                    O)\n                    <jats:sub>6<\/jats:sub>\n                    ][P\n                    <jats:sub>2<\/jats:sub>\n                    W\n                    <jats:sub>17<\/jats:sub>\n                    V\n                    <jats:sub>1<\/jats:sub>\n                    O\n                    <jats:sub>62<\/jats:sub>\n                    ] denoted as XMOF\u2010V\n                    <jats:sub>1<\/jats:sub>\n                    (X = Fe; Co; Zn, DPYB = 1,4\u2010Di(pyridin\u20104\u2010yl)benzene, OX = oxalic acid). The incorporation of P\n                    <jats:sub>2<\/jats:sub>\n                    W\n                    <jats:sub>17<\/jats:sub>\n                    V\n                    <jats:sub>1<\/jats:sub>\n                    not only reinforced structural ruggedness and stability, but also promotes multi\u2010electron transfer, substantially promoting e\u2010NO\n                    <jats:sub>3<\/jats:sub>\n                    RA activity. Among them FeMOF\u2010V\n                    <jats:sub>1<\/jats:sub>\n                    delivers exceptional electrocatlytic nitrat\u2010to\u2010ammonia performance with an achieves over 95% Faradaic efficiency across a wide voltage range of \u22120.6 to \u22121.4\u00a0V vs RHE. This superiority stems from synergistic interplay: P\n                    <jats:sub>2<\/jats:sub>\n                    W\n                    <jats:sub>17<\/jats:sub>\n                    V\n                    <jats:sub>1<\/jats:sub>\n                    acts as an electron reservoir enhancing proton\u2010coupled charge transfer, while the minimal bandgap of FeMOF\u2010V\n                    <jats:sub>1<\/jats:sub>\n                    facilitates directional electron injection. DFT analyses reveal Fe\u2010specific mechanisms including strong 3\n                    <jats:italic>d<\/jats:italic>\n                    \u2010orbital hybridization with NO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2013<\/jats:sup>\n                    near Fermi Level (Ef), highly positive Fe sites optimizing adsorption, and transfer weakening N\u2013O bonds, as corroborated by in situ FTIR identification of *NO\n                    <jats:sub>3<\/jats:sub>\n                    \/*NO\/*NH\n                    <jats:sub>2<\/jats:sub>\n                    intermediates. Together with effectively suppressed HER (\u0394G\n                    <jats:sub>*H<\/jats:sub>\n                    &gt; \u0394G\n                    <jats:sub>*NO3<\/jats:sub>\n                    ), these attributes collectively enable highly selective NH\n                    <jats:sub>3<\/jats:sub>\n                    synthesis. This study establishes mixed\u2010addenda POMOFs as a versatile and efficient platform for sustainable nitrate\u2010to\u2010ammonia conversion.\n                  <\/jats:p>","DOI":"10.1002\/advs.202521317","type":"journal-article","created":{"date-parts":[[2025,12,26]],"date-time":"2025-12-26T06:02:57Z","timestamp":1766728977000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":12,"title":["Molecular Weaving of Mixed\u2010Addenda Polyoxometalates into MOF Nanochannels as Electron\u2010Buffering Reservoirs for Enhanced Nitrate\u2010to\u2010Ammonia Electrocatalysis"],"prefix":"10.1002","volume":"13","author":[{"given":"Gang","family":"Li","sequence":"first","affiliation":[{"name":"School of Materials Science and Chemical Engineering Harbin University of Science and Technology  Harbin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5418-9182","authenticated-orcid":false,"given":"Xinming","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Chemical Engineering Harbin University of Science and Technology  Harbin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haijun","family":"Pang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Chemical Engineering Harbin University of Science and Technology  Harbin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huiyuan","family":"Ma","sequence":"additional","affiliation":[{"name":"School of Materials Science and Chemical Engineering Harbin University of Science and Technology  Harbin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,12,25]]},"reference":[{"key":"e_1_2_9_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.nanoen.2020.105126"},{"key":"e_1_2_9_3_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2022.121574"},{"key":"e_1_2_9_4_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2021.121021"},{"key":"e_1_2_9_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/acssuschemeng.1c07824"},{"key":"e_1_2_9_6_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-021-23115-x"},{"key":"e_1_2_9_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.2c02048"},{"key":"e_1_2_9_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.1c21691"},{"key":"e_1_2_9_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202001267"},{"key":"e_1_2_9_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.201901627"},{"key":"e_1_2_9_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202202604"},{"key":"e_1_2_9_12_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jechem.2021.01.039"},{"key":"e_1_2_9_13_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c07762"},{"key":"e_1_2_9_14_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-021-00599-w"},{"key":"e_1_2_9_15_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2022.135104"},{"key":"e_1_2_9_16_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202010052"},{"key":"e_1_2_9_17_1","doi-asserted-by":"publisher","DOI":"10.1039\/C7TA10866D"},{"key":"e_1_2_9_18_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41565-022-01121-4"},{"key":"e_1_2_9_19_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.0c22338"},{"key":"e_1_2_9_20_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202008533"},{"key":"e_1_2_9_21_1","doi-asserted-by":"publisher","DOI":"10.1039\/D1TA05718A"},{"key":"e_1_2_9_22_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202107858"},{"key":"e_1_2_9_23_1","doi-asserted-by":"publisher","DOI":"10.1039\/D1GC01913A"},{"key":"e_1_2_9_24_1","doi-asserted-by":"publisher","DOI":"10.1093\/nsr\/nwz019"},{"key":"e_1_2_9_25_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.2c03452"},{"key":"e_1_2_9_26_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202004523"},{"key":"e_1_2_9_27_1","first-page":"2092","article-title":"Accelerating 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