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Here, isomeric Cu(I) triazolate frameworks (MAF\u20102Fa and MAF\u20102Fb) with similar thermal\/chemical stabilities but very different coordination modes are used for eCO<jats:sub>2<\/jats:sub>RR studies. MAF\u20102Fa with monotypic planar dinuclear Cu(I) coordination mode achieves high selectivity for C<jats:sub>2<\/jats:sub>H<jats:sub>4<\/jats:sub> (53%) and C<jats:sub>2<\/jats:sub> products (70%), with almost unchanged over a wide potential window (\u20121.1 to \u20121.5\u00a0V), making it among one of the best Cu\u2010complex electrocatalysts. In contrast, MAF\u20102Fb with multiple Cu(I) coordination modes (including planar\/bent dinuclear, linear mononuclear, and trigonal mononuclear ones) showed low C<jats:sub>2<\/jats:sub>\/C<jats:sub>1<\/jats:sub> products without significant differences. More interestingly, MAF\u20102Fa can maintain its performance for at least 8 h, whereas MAF\u20102Fb decomposed into inorganics with inferior performance after 1.5 h. The significant differences of eCO<jats:sub>2<\/jats:sub>RR selectivities and stabilities are elucidated by computational simulations and operando electrochemical tests.<\/jats:p>","DOI":"10.1002\/smll.202408510","type":"journal-article","created":{"date-parts":[[2024,12,13]],"date-time":"2024-12-13T04:57:47Z","timestamp":1734065867000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["Isomeric Cu(I) Azolate Frameworks Showing Contrasting Electrocatalytic CO<sub>2<\/sub> Reduction Selectivities and Stabilities"],"prefix":"10.1002","volume":"21","author":[{"given":"Kai","family":"Zheng","sequence":"first","affiliation":[{"name":"MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular Engineering School of Chemistry IGCME Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ding\u2010Yi","family":"Hu","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular Engineering School of Chemistry IGCME Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chao","family":"Wang","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular Engineering School of Chemistry IGCME Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zi\u2010Jun","family":"Liang","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular Engineering School of Chemistry IGCME Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xue\u2010Wen","family":"Zhang","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular Engineering School of Chemistry IGCME Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xian\u2010Xian","family":"Xiao","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular Engineering School of Chemistry IGCME Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jun\u2010Xi","family":"Wu","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular Engineering School of Chemistry IGCME Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lin\u2010Ling","family":"Zhuo","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular Engineering School of Chemistry IGCME Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Duo\u2010Yu","family":"Lin","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular Engineering School of Chemistry IGCME Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1105-8702","authenticated-orcid":false,"given":"Dong\u2010Dong","family":"Zhou","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular Engineering School of Chemistry IGCME Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jie\u2010Peng","family":"Zhang","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular Engineering School of Chemistry IGCME Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,12,12]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jechem.2023.08.042"},{"key":"e_1_2_8_1_2","doi-asserted-by":"publisher","DOI":"10.1021\/acsenergylett.7b00621"},{"key":"e_1_2_8_1_3","doi-asserted-by":"publisher","DOI":"10.1016\/j.isci.2022.104177"},{"key":"e_1_2_8_1_4","volume":"41","author":"Wan C.\u2010P.","year":"2022","journal-title":"Chin. 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