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To address this challenge, the creatively spatial electronic partitioning is proposed to promote the intermediate proximity and thus facilitate efficient CO2 activation and distance-governed C\u2013C coupling. The feasibility of this strategy is demonstrated in a series of copper-tetrazole metal\u2013organic frameworks (MOFs, Cu-Tz-X, X = F, Cl, Br), which integrates coexisting free and halogen-confined cages. Within halogen-confined cages, the multidentate aromatic \u03c0 faces cooperatively stabilize X anions through chelation-like noncovalent X\u00b7\u00b7\u00b7\u03c0 interactions, polarizing the adjacent Tz linker into electrophilic domains while redistributing nucleophilic Cu sites. The halogen-induced electrophile\u2013nucleophile electronic partition simultaneously promotes dual-site CO2 bending activation and enforces an optimal short-range *CO*CHO coupling distance, as evidenced by X-ray absorption spectroscopy, in situ FT-IR and theoretical simulations. Compared with halogen-free Cu-Tz-NO3, optimized Cu-Tz-Cl exhibits a reduced activation barrier, 10-fold enhancement in the C\u2013C coupling rate, and a broad pH range catalytic stability. Remarkably, it maintains a high C2H4 FE of \u223c61.3% even in a strongly acidic bulk electrolyte (pH = 1) at a total current density of 469 mA cm\u20132, outperforming previously reported MOF-based materials. This spatial electronic partitioning strategy establishes a well-defined catalytic microenvironment in confined catalytic systems toward efficient CO2 reduction.<\/jats:p>","DOI":"10.1021\/jacs.6c06810","type":"journal-article","created":{"date-parts":[[2026,8,31]],"date-time":"2026-08-31T09:34:09Z","timestamp":1788168849000},"page":"36662-36674","source":"Crossref","is-referenced-by-count":1,"title":["Spatial Electronic\nPartitioning in Metal\u2013Organic\nFrameworks for pH-Universal CO2 Electroreduction"],"prefix":"10.1021","volume":"148","author":[{"given":"Jie","family":"Meng","sequence":"first","affiliation":[{"name":"Shaanxi Normal University , , , ,","place":["Xi\u2019an, Shaanxi, China, 710062"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6199-6783","authenticated-orcid":true,"given":"Ying","family":"Wang","sequence":"additional","affiliation":[{"name":"Shaanxi Normal University , , , ,","place":["Xi\u2019an, Shaanxi, China, 710062"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jia-Wen","family":"Wang","sequence":"additional","affiliation":[{"name":"Shaanxi Normal University , , , ,","place":["Xi\u2019an, Shaanxi, China, 710062"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ze-Lin","family":"Ma","sequence":"additional","affiliation":[{"name":"Northwestern Polytechnical University and Shaanxi Joint Laboratory of Graphene (NPU) , , , ,","place":["Xi\u2019an, Shaanxi, China, 710072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tian-Shu","family":"He","sequence":"additional","affiliation":[{"name":"Shaanxi Normal University , , , ,","place":["Xi\u2019an, Shaanxi, China, 710062"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiao-Na","family":"Yue","sequence":"additional","affiliation":[{"name":"Shaanxi Normal University , , , ,","place":["Xi\u2019an, Shaanxi, China, 710062"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bo-Lin","family":"Sun","sequence":"additional","affiliation":[{"name":"Shaanxi Normal University , , , ,","place":["Xi\u2019an, Shaanxi, China, 710062"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1117-4017","authenticated-orcid":true,"given":"Quan-Guo","family":"Zhai","sequence":"additional","affiliation":[{"name":"Shaanxi Normal University , , , ,","place":["Xi\u2019an, Shaanxi, China, 710062"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,24]]},"reference":[{"issue":"21","key":"2026090312080299200_cit1","doi-asserted-by":"publisher","first-page":"10156","DOI":"10.1039\/D5CS00780A","article-title":"Optimizing CO2 electroreduction:\ntheoretical insights for enhancing efficiency across elementary steps","volume":"54","author":"Wang","year":"2025","journal-title":"Chem. 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