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However, the mechanism and potential limitations remain poorly understood. Here we report that subtle changes in molecular configurations can profoundly affect, conducively or adversely, the catalytic selectivity and product turnover frequencies (TOFs) of CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction reaction. Specifically, introducing molecular curvature in cobalt tetraaminophthalocyanine improves the multielectron reduction activity by favorable *CO hydrogenation, attaining methanol Faradaic efficiency up to 52\u2009%. In stark contrast, strained iron phthalocyanine exacerbates *CO poisoning, leading to decreased TOF\n                    <jats:sub>CO<\/jats:sub>\n                    by &gt;50\u2009% at \u22120.5\u2005V\n                    <jats:sub>RHE<\/jats:sub>\n                    and a rapid current decay. The uniform dispersion is crucial for optimizing electron transfer, while activity is distinctly sensitive to the local atomic environment around the active sites. Specifically, local strain either enhances binding to intermediates or poisons the catalytic sites. Our comprehensive analysis elucidates the intricate relationship between molecular structure and activities, offering insights into designing efficient heterogeneous molecular interfaces.\n                  <\/jats:p>","DOI":"10.1002\/anie.202420286","type":"journal-article","created":{"date-parts":[[2024,11,25]],"date-time":"2024-11-25T11:08:58Z","timestamp":1732532938000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":28,"title":["Subtle Modifications in Interface Configurations of Iron\/Cobalt Phthalocyanine\u2010Based Electrocatalysts Determine Molecular CO\n                    <sub>2<\/sub>\n                    Reduction Activities"],"prefix":"10.1002","volume":"64","author":[{"given":"Yinger","family":"Xin","sequence":"first","affiliation":[{"name":"Department of Chemistry State Key Laboratory of Marine Pollution City University of Hong Kong  Tat Chee Avenue 83 Kowloon Hong Kong SAR 999077 P. R. 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