{"title":"咪唑配体修饰的Cu2O催化剂通过局部*CO富集增强CO2电还原中C2+的选择性","authors":"Rongzhen Chen, Ling Zhang and Yuhang Li","doi":"10.1039/D5IM00052A","DOIUrl":null,"url":null,"abstract":"<p>Electrochemical CO<small><sub>2</sub></small> reduction (CO<small><sub>2</sub></small>RR) to synthesize multicarbon products is a critical route for sustainable CO<small><sub>2</sub></small> utilization, yet achieving high selectivity and current density simultaneously remains challenging. While enhancing *CO coverage on catalysts is pivotal for promoting C–C coupling, the dynamic competition between intermediate enrichment and microenvironment regulation necessitates innovative strategies. Here, we employ surface ligand engineering to construct a tunable hydrophobic microenvironment on Cu<small><sub>2</sub></small>O catalysts, using imidazolium-based ionic liquids with alkyl side chains of varying lengths. The optimized OMIm-Cu<small><sub>2</sub></small>O catalyst achieves a C<small><sub>2+</sub></small> selectivity of 63.3% in alkaline media and 30.7% in acidic media. Mechanistic studies reveal that hydrophobic long-chain ligands elevate local *CO concentration, facilitating efficient C–C coupling. This work highlights microenvironment modulation as a viable pathway to bridge the gap between high efficiency and industria–current–density performance in CO<small><sub>2</sub></small>RR.</p><p>Keywords: Electrochemical CO<small><sub>2</sub></small> reduction; C<small><sub>2+</sub></small> product selectivity; Copper-based catalysts; *CO concentration.</p>","PeriodicalId":29808,"journal":{"name":"Industrial Chemistry & Materials","volume":" 4","pages":" 431-439"},"PeriodicalIF":0.0000,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/im/d5im00052a?page=search","citationCount":"0","resultStr":"{\"title\":\"Imidazolium ligand-modified Cu2O catalysts for enhancing C2+ selectivity in CO2 electroreduction via local *CO enrichment†\",\"authors\":\"Rongzhen Chen, Ling Zhang and Yuhang Li\",\"doi\":\"10.1039/D5IM00052A\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Electrochemical CO<small><sub>2</sub></small> reduction (CO<small><sub>2</sub></small>RR) to synthesize multicarbon products is a critical route for sustainable CO<small><sub>2</sub></small> utilization, yet achieving high selectivity and current density simultaneously remains challenging. While enhancing *CO coverage on catalysts is pivotal for promoting C–C coupling, the dynamic competition between intermediate enrichment and microenvironment regulation necessitates innovative strategies. Here, we employ surface ligand engineering to construct a tunable hydrophobic microenvironment on Cu<small><sub>2</sub></small>O catalysts, using imidazolium-based ionic liquids with alkyl side chains of varying lengths. The optimized OMIm-Cu<small><sub>2</sub></small>O catalyst achieves a C<small><sub>2+</sub></small> selectivity of 63.3% in alkaline media and 30.7% in acidic media. Mechanistic studies reveal that hydrophobic long-chain ligands elevate local *CO concentration, facilitating efficient C–C coupling. This work highlights microenvironment modulation as a viable pathway to bridge the gap between high efficiency and industria–current–density performance in CO<small><sub>2</sub></small>RR.</p><p>Keywords: Electrochemical CO<small><sub>2</sub></small> reduction; C<small><sub>2+</sub></small> product selectivity; Copper-based catalysts; *CO concentration.</p>\",\"PeriodicalId\":29808,\"journal\":{\"name\":\"Industrial Chemistry & Materials\",\"volume\":\" 4\",\"pages\":\" 431-439\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2025-05-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://pubs.rsc.org/en/content/articlepdf/2025/im/d5im00052a?page=search\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Industrial Chemistry & Materials\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2025/im/d5im00052a\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Industrial Chemistry & Materials","FirstCategoryId":"1085","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2025/im/d5im00052a","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Imidazolium ligand-modified Cu2O catalysts for enhancing C2+ selectivity in CO2 electroreduction via local *CO enrichment†
Electrochemical CO2 reduction (CO2RR) to synthesize multicarbon products is a critical route for sustainable CO2 utilization, yet achieving high selectivity and current density simultaneously remains challenging. While enhancing *CO coverage on catalysts is pivotal for promoting C–C coupling, the dynamic competition between intermediate enrichment and microenvironment regulation necessitates innovative strategies. Here, we employ surface ligand engineering to construct a tunable hydrophobic microenvironment on Cu2O catalysts, using imidazolium-based ionic liquids with alkyl side chains of varying lengths. The optimized OMIm-Cu2O catalyst achieves a C2+ selectivity of 63.3% in alkaline media and 30.7% in acidic media. Mechanistic studies reveal that hydrophobic long-chain ligands elevate local *CO concentration, facilitating efficient C–C coupling. This work highlights microenvironment modulation as a viable pathway to bridge the gap between high efficiency and industria–current–density performance in CO2RR.
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