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However, this kinetically challenging eight\u2010electron multistep deep\u2010reduction encounters insufficient catalyst design principles to steer complex CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction pathways. Utilizing atomic copper (Cu) structures with unitary active sites can boost eCO\n                    <jats:sub>2<\/jats:sub>\n                    R\u2010to\u2010CH\n                    <jats:sub>4<\/jats:sub>\n                    selectivity due to the efficient suppression of unwanted C\u2500C coupling. Herein, we report a sequential ion exchange strategy to fabricate periodic Cu single\u2010atom catalysts within a polymeric carbon nitride (PCN) matrix, where the uniformly dispersed, diagonally coordinated N\u2500Cu\u2500N configuration hosts low\u2010valent Cu\n                    <jats:sup>\u03b4+<\/jats:sup>\n                    centers. Leveraging the periodic N\u2010anchoring sites with delocalized \u03c0\u2010electron conjugation in the PCN matrix, the isolated Cu sites are obtained with an interatomic distance of \u223c4.2\u00a0\u00c5 under high metal\u2010loading conditions. This engineered spatial configuration effectively inhibits C\u2500C coupling to avoid subsequent multicarbon product formation. The optimized Cu\n                    <jats:sub>1<\/jats:sub>\n                    \/PCN demonstrates exceptional eCO\n                    <jats:sub>2<\/jats:sub>\n                    R\u2010to\u2010CH\n                    <jats:sub>4<\/jats:sub>\n                    performance, achieving 71.1% CH\n                    <jats:sub>4<\/jats:sub>\n                    Faradaic efficiency with a high partial current density of 426.6\u00a0mA\u00a0cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    at \u22121.50\u00a0V versus reversible hydrogen electrode, outpacing the state\u2010of\u2010the\u2010art catalysts. This work delves into effective concepts for steering desirable reaction pathways via precisely modulating active site structures at the atomic level to create favorable microenvironments.\n                  <\/jats:p>","DOI":"10.1002\/anie.202508497","type":"journal-article","created":{"date-parts":[[2025,5,12]],"date-time":"2025-05-12T04:05:08Z","timestamp":1747022708000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":20,"title":["Engineered Spatial Confinement of Cu Single\u2010Atoms with Diagonal N\u2500Cu\u2500N Motifs for High\u2010Rate CO\n                    <sub>2<\/sub>\n                    Methanation"],"prefix":"10.1002","volume":"64","author":[{"given":"Guanghui","family":"Feng","sequence":"first","affiliation":[{"name":"Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological Engineering Zhejiang University  Hangzhou 310027 China"},{"name":"Institute of Zhejiang 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