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Herein, three\u2010 and four\u2010nitrogen\u2010coordinated Cu single\u2010atom motifs, denoted as Cu\u2500N\n                    <jats:sub>3<\/jats:sub>\n                    and Cu\u2500N\n                    <jats:sub>4<\/jats:sub>\n                    , are constructed as well\u2010defined pre\u2010catalyst models to elucidate how the initial Cu coordination environment directs pH\u2010dependent active\u2010site reconstruction.\n                    <jats:italic>Operando<\/jats:italic>\n                    X\u2010ray absorption spectroscopy and wavelet\u2010transform EXAFS reveal that Cu\u2500N\n                    <jats:sub>4<\/jats:sub>\n                    readily undergoes rapid reconstruction under acidic, neutral, and alkaline conditions, generating low\u2010coordinated, electron\u2010enriched Cu species while concomitantly inducing Cu\u2500Cu aggregation and excessive Cu\u2500site reduction. In contrast, Cu\u2500N\n                    <jats:sub>3<\/jats:sub>\n                    displays more regulated site evolution, with limited activation under acidic conditions but progressive formation of low\u2010coordinated Cu\u2500N\n                    <jats:sub>x<\/jats:sub>\n                    active structures under neutral and alkaline conditions. In situ ATR\u2010FTIR further verifies that the dynamically evolved Cu\u2500N\n                    <jats:sub>3<\/jats:sub>\n                    sites enhance nitrate adsorption, facilitate N\u2500O bond activation, and promote the formation of hydrogenated nitrogen intermediates. These findings establish coordination\u2010governed site evolution as a design principle for balancing productive Cu\u2500site activation and metal\u2010centered over\u2010reduction, providing molecular\u2010level guidance for the design of pH\u2010adaptive NO\n                    <jats:sub>3<\/jats:sub>\n                    RR catalysts.\n                  <\/jats:p>","DOI":"10.1002\/advs.78164","type":"journal-article","created":{"date-parts":[[2026,10,15]],"date-time":"2026-10-15T03:29:48Z","timestamp":1792034988000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Coordination\u2010Asymmetry\u2010Regulated Reconstruction of Electron\u2010Rich Cu Sites for pH\u2010Dependent Nitrate\u2010to\u2010Ammonia 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