Zhihao Nie, Licheng Yu, Lili Jiang, Ming Li, Shan Ding, Baokai Xia, Chi Cheng, Jingjing Duan, Sheng Chen
{"title":"二氧化碳电还原制甲酸盐的金属有机骨架(MOF)厚度控制","authors":"Zhihao Nie, Licheng Yu, Lili Jiang, Ming Li, Shan Ding, Baokai Xia, Chi Cheng, Jingjing Duan, Sheng Chen","doi":"10.1002/cnl2.66","DOIUrl":null,"url":null,"abstract":"<p>Decreasing particle size (like thickness) is a common strategy to enhance the activities of catalysts. In this work, we have synthesized two coppers, which are bismuth-based metal-organic framework (CuBi-MOF) catalysts with different thicknesses (134.8 and 2.0 nm). In contrast to common expectations, large thickness CuBi-MOF has exhibited superior activities as a comparison to its small-thickness counterpart in terms of carbon dioxide electroreduction to produce formate, characteristic of high selectivity (Faraday efficiency > 90%), a wide window of potential (−0.6 to −1.6 V vs. reversible hydrogen electrode), and large current densities (up to −380 mA cm<sup>−2</sup>). The mechanism study has been performed by using density functional theory calculations, which highlight the strong synergic effect between Cu and Bi sites in large-thickness CuBi-MOF for activating CO<sub>2</sub> molecules. Consequently, large-thickness CuBi-MOF could show smaller Gibbs free energies compared to its small counterpart for binding with reaction intermediate (*COOH, 1.1 vs. 1.8 eV). The result of this work could provide new insights into catalyst design toward a number of electrochemical systems.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":null,"pages":null},"PeriodicalIF":0.0000,"publicationDate":"2023-06-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.66","citationCount":"0","resultStr":"{\"title\":\"Metal-organic framework (MOF) thickness control for carbon dioxide electroreduction to formate\",\"authors\":\"Zhihao Nie, Licheng Yu, Lili Jiang, Ming Li, Shan Ding, Baokai Xia, Chi Cheng, Jingjing Duan, Sheng Chen\",\"doi\":\"10.1002/cnl2.66\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Decreasing particle size (like thickness) is a common strategy to enhance the activities of catalysts. In this work, we have synthesized two coppers, which are bismuth-based metal-organic framework (CuBi-MOF) catalysts with different thicknesses (134.8 and 2.0 nm). In contrast to common expectations, large thickness CuBi-MOF has exhibited superior activities as a comparison to its small-thickness counterpart in terms of carbon dioxide electroreduction to produce formate, characteristic of high selectivity (Faraday efficiency > 90%), a wide window of potential (−0.6 to −1.6 V vs. reversible hydrogen electrode), and large current densities (up to −380 mA cm<sup>−2</sup>). The mechanism study has been performed by using density functional theory calculations, which highlight the strong synergic effect between Cu and Bi sites in large-thickness CuBi-MOF for activating CO<sub>2</sub> molecules. Consequently, large-thickness CuBi-MOF could show smaller Gibbs free energies compared to its small counterpart for binding with reaction intermediate (*COOH, 1.1 vs. 1.8 eV). The result of this work could provide new insights into catalyst design toward a number of electrochemical systems.</p>\",\"PeriodicalId\":100214,\"journal\":{\"name\":\"Carbon Neutralization\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2023-06-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.66\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Carbon Neutralization\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/cnl2.66\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Carbon Neutralization","FirstCategoryId":"1085","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/cnl2.66","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Metal-organic framework (MOF) thickness control for carbon dioxide electroreduction to formate
Decreasing particle size (like thickness) is a common strategy to enhance the activities of catalysts. In this work, we have synthesized two coppers, which are bismuth-based metal-organic framework (CuBi-MOF) catalysts with different thicknesses (134.8 and 2.0 nm). In contrast to common expectations, large thickness CuBi-MOF has exhibited superior activities as a comparison to its small-thickness counterpart in terms of carbon dioxide electroreduction to produce formate, characteristic of high selectivity (Faraday efficiency > 90%), a wide window of potential (−0.6 to −1.6 V vs. reversible hydrogen electrode), and large current densities (up to −380 mA cm−2). The mechanism study has been performed by using density functional theory calculations, which highlight the strong synergic effect between Cu and Bi sites in large-thickness CuBi-MOF for activating CO2 molecules. Consequently, large-thickness CuBi-MOF could show smaller Gibbs free energies compared to its small counterpart for binding with reaction intermediate (*COOH, 1.1 vs. 1.8 eV). The result of this work could provide new insights into catalyst design toward a number of electrochemical systems.