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Herein, we synthesize a polyphosphazene network with a precise supramolecular configuration of the neighboring dual catalytic centers by introducing dendritic molecules. The reasonable ratio of 5,10,15,20\u2010tetrakis\u2010(4\u2010aminophenyl)\u2010porphyrin\u2010Cu\u2010(II) and hexachlorocyclotriphosphazene results in an ultrathin polymer sheath around carbon nanotubes, exhibiting \u03c0\u2013\u03c0 stacking between the adjacent porphyrin molecules and the optimized spatial distance (3.8 \u00c5) between the neighboring Cu active sites, featuring dual\u2010atom catalytic centers bound to carbon nanotubes. Given the controlled geometric structure, the catalysts can boost C\u2500C coupling reactions during CO\n                    <jats:sub>2<\/jats:sub>\n                    electrocatalysis, thereby improving the selectivity of the multi\u2010carbon product (EtOH) with a high Faradic efficiency (FE\n                    <jats:sub>max<\/jats:sub>\n                    of 61.1% at \u22121.0\u00a0V) in broad potential windows. The strategy of achieving precise control over the spatial distance between adjacent metal catalytic centers by incorporating dendritic molecules into a polyphosphazene network provides a viable approach for designing polymer\u2010based single\u2010atom electrocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/smll.74922","type":"journal-article","created":{"date-parts":[[2026,8,3]],"date-time":"2026-08-03T07:26:31Z","timestamp":1785741991000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Spatially Engineered Cu(II)\u2010Containing Polyphosphazene\u2010Based Catalysts Enable Electrochemical CO\n                    <sub>2<\/sub>\n                    Reduction to Ethanol"],"prefix":"10.1002","volume":"22","author":[{"given":"Shujing","family":"Liu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular Science Fudan University  Shanghai China"},{"name":"State Key Laboratory of Space Power Sources Shanghai Institute of Space Power\u2010Sources  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wanting","family":"Xie","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular Science Fudan University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinyao","family":"Zhu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular Science Fudan University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pinit","family":"Kidkhunthod","sequence":"additional","affiliation":[{"name":"Synchrotron Light Research Institute 111 University Avenue  Nakhon Ratchasima 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