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Herein, we report a mechanochemically assisted synthesis of high\u2010density tin single\u2010site catalysts, in which atomically dispersed Sn centers are stabilized at loadings of approximately 7.5\u00a0wt.%, exceeding the typical \u223c2\u00a0wt.% limit reported for Sn single\u2010site systems without detectable aggregation. By tailoring the nitrogen\u2010rich precursor chemistry, catalysts with distinct coordination environments and controlled site densities were obtained, providing a platform to elucidate how these two factors govern the CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction pathway. Operando spectroscopy combined with density functional theory reveals that the local coordination environment governs intrinsic activity and selectivity by stabilizing key intermediates along the *OCHO pathway, whereas the mechanochemical process primarily enhances the density of electrochemically accessible Sn sites. The optimized catalyst achieves formate Faradaic efficiencies above 90% over a wide current\u2010density range of 50\u2013500\u00a0mA\u00a0cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    in a gas\u2010fed flow cell, reaching 92.5% at 100\u00a0mA\u00a0cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , and maintains stable operation for over 100\u00a0h at 100\u00a0mA\u00a0cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    . This work provides mechanistic insights and design principles for selective and high\u2010rate CO\n                    <jats:sub>2<\/jats:sub>\n                    electroreduction based on single\u2010site catalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.7872408","type":"journal-article","created":{"date-parts":[[2026,8,27]],"date-time":"2026-08-27T08:47:16Z","timestamp":1787820436000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Maximizing Active Site Density in Tin Single\u2010Site Catalysts for Selective Carbon Dioxide to Formate Electroreduction"],"prefix":"10.1002","volume":"65","author":[{"given":"Katharina","family":"Potemkin","sequence":"first","affiliation":[{"name":"Department of Chemistry Johannes Gutenberg University Mainz  Mainz 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