{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,19]],"date-time":"2026-09-19T16:06:34Z","timestamp":1789833994202,"version":"4.0.1"},"reference-count":52,"publisher":"Wiley","license":[{"start":{"date-parts":[[2026,9,19]],"date-time":"2026-09-19T00:00:00Z","timestamp":1789776000000},"content-version":"vor","delay-in-days":0,"URL":"http:\/\/creativecommons.org\/licenses\/by\/4.0\/"},{"start":{"date-parts":[[2026,9,19]],"date-time":"2026-09-19T00:00:00Z","timestamp":1789776000000},"content-version":"tdm","delay-in-days":0,"URL":"http:\/\/doi.wiley.com\/10.1002\/tdm_license_1.1"}],"content-domain":{"domain":["onlinelibrary.wiley.com"],"crossmark-restriction":true},"short-container-title":["Angew Chem Int Ed"],"abstract":"<jats:title>ABSTRACT<\/jats:title>\n                  <jats:p>\n                    Developing electrocatalysts with active sites that undergo structural evolution under operating conditions remains a challenge in electrochemical nitrate reduction. Here, we use single\u2010crystalline mesoporous metal\u2013organic frameworks (MOFs) with distinct pore geometries to investigate the potential\u2010dependent evolution of iron active sites during electrochemical nitrate\u2010to\u2010ammonia conversion. Fe single atoms are anchored within hexagonal and cubic mesoporous frameworks, providing two structurally distinct environments for examining their catalytic and working\u2010state responses.\n                    <jats:italic>Operando<\/jats:italic>\n                    FTIR, H\/D isotope\u2010exchange, and DRT analyses reveal that the 1D hexagonal mesoporous environment is associated with a distinct interfacial\u2010water response and proton\u2010involved reaction behavior. This response coincides with changes in the average Fe coordination environment.\n                    <jats:italic>Operando<\/jats:italic>\n                    XAS further reveals potential\u2010dependent changes in both catalysts, with FeSAs@\n                    <jats:italic>m<\/jats:italic>\n                    UiO\u2010P exhibiting a more pronounced Fe\u2010associated higher\u2010shell contribution and greater post\u2010potential recovery. Under the investigated conditions, FeSAs@\n                    <jats:italic>m<\/jats:italic>\n                    UiO\u2010P achieves a Faradaic efficiency of 99.1% at \u22121.05\u00a0V versus RHE and exhibits higher NH\n                    <jats:sub>3<\/jats:sub>\n                    selectivity than its cubic counterpart. Collectively, these findings reveal a potential\u2010dependent correspondence among mesopore architecture, interfacial water organization, and Fe\u2010site evolution. Although the causal relationship between water organization and Fe\u2010site evolution remains to be established, this correspondence provides a working framework for investigating reaction\u2010state\u2010dependent catalytic interfaces.\n                  <\/jats:p>","DOI":"10.1002\/anie.5865467","type":"journal-article","created":{"date-parts":[[2026,9,19]],"date-time":"2026-09-19T15:49:06Z","timestamp":1789832946000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Coordinating Mesopore Geometry and Interfacial Water Dynamics for Iron\u2010Site Evolution in Nitrate Electroreduction"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0000-2809-7957","authenticated-orcid":false,"given":"Xiangyang","family":"Liu","sequence":"first","affiliation":[{"name":"Department of Materials Process Engineering, Graduate School of Engineering Nagoya University  Nagoya 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Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0590-1396","authenticated-orcid":false,"given":"Kevin C.\u2010W.","family":"Wu","sequence":"additional","affiliation":[{"name":"Molecular Science and Technology Program Taiwan International Graduate Program Academia Sinica  Taipei Taiwan"},{"name":"International Graduate Program of Molecular Science and Technology (NTU\u2010MST) National Taiwan University  Taipei Taiwan"},{"name":"Department of Chemical Engineering National Taiwan University  Taipei Taiwan"},{"name":"Center of Atomic Initiative for New Materials (AI\u2010MAT) National Taiwan University  Taipei Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9785-5061","authenticated-orcid":false,"given":"Ho Ngoc","family":"Nam","sequence":"additional","affiliation":[{"name":"Department of Materials Process Engineering, Graduate School of Engineering Nagoya University  Nagoya 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