Shilei Wei , Hang Hua , Qingxuan Ren , Jingshan Luo
{"title":"通过硅酸盐缓冲层增强酸性电解质膜电极组件的二氧化碳电化学还原能力","authors":"Shilei Wei , Hang Hua , Qingxuan Ren , Jingshan Luo","doi":"10.1016/S1872-2067(24)60129-4","DOIUrl":null,"url":null,"abstract":"<div><div>The electrochemical reduction of CO<sub>2</sub> holds considerable promise in combating global climate change while yielding valuable chemical commodities. Membrane electrode assemblies operating within acidic electrolyte have exhibited noteworthy advancements in CO<sub>2</sub> utilization efficiency, albeit encountering formidable competition from the hydrogen evolution reaction. In our investigation, we introduced a silicate buffer layer, which yielded exceptional outcomes even using strong acid electrolyte. Notably, our approach yielded a CO Faradic efficiency of 90% and reached a substantial current density of 400 mA cm<sup>–2</sup>. Furthermore, our system displayed remarkable stability over a 12-hour duration, and achieved a high single-pass-conversion efficiency of 67%. Leveraging <em>in-situ</em> Raman analysis, we attributed these performance enhancements to the augmented CO<sub>2</sub> adsorption and localized alkaline environment facilitated by the incorporation of the silicate buffer layer. We think the addition of buffer layer to adjust the microenvironment is essential to achieve high performance and keep stable in acid condition.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"66 ","pages":"Pages 139-145"},"PeriodicalIF":15.7000,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhanced electrochemical carbon dioxide reduction in membrane electrode assemblies with acidic electrolytes through a silicate buffer layer\",\"authors\":\"Shilei Wei , Hang Hua , Qingxuan Ren , Jingshan Luo\",\"doi\":\"10.1016/S1872-2067(24)60129-4\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The electrochemical reduction of CO<sub>2</sub> holds considerable promise in combating global climate change while yielding valuable chemical commodities. Membrane electrode assemblies operating within acidic electrolyte have exhibited noteworthy advancements in CO<sub>2</sub> utilization efficiency, albeit encountering formidable competition from the hydrogen evolution reaction. In our investigation, we introduced a silicate buffer layer, which yielded exceptional outcomes even using strong acid electrolyte. Notably, our approach yielded a CO Faradic efficiency of 90% and reached a substantial current density of 400 mA cm<sup>–2</sup>. Furthermore, our system displayed remarkable stability over a 12-hour duration, and achieved a high single-pass-conversion efficiency of 67%. Leveraging <em>in-situ</em> Raman analysis, we attributed these performance enhancements to the augmented CO<sub>2</sub> adsorption and localized alkaline environment facilitated by the incorporation of the silicate buffer layer. We think the addition of buffer layer to adjust the microenvironment is essential to achieve high performance and keep stable in acid condition.</div></div>\",\"PeriodicalId\":9832,\"journal\":{\"name\":\"Chinese Journal of Catalysis\",\"volume\":\"66 \",\"pages\":\"Pages 139-145\"},\"PeriodicalIF\":15.7000,\"publicationDate\":\"2024-11-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chinese Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1872206724601294\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chinese Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1872206724601294","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
引用次数: 0
摘要
二氧化碳的电化学还原在应对全球气候变化方面大有可为,同时还能产生宝贵的化工产品。在酸性电解质中运行的膜电极组件在二氧化碳利用效率方面取得了显著进步,尽管遇到了氢进化反应的激烈竞争。在我们的研究中,我们引入了硅酸盐缓冲层,即使使用强酸电解质也能产生卓越的效果。值得注意的是,我们的方法产生了 90% 的二氧化碳法拉第效率,并达到了 400 mA cm-2 的巨大电流密度。此外,我们的系统在 12 小时的持续时间内表现出卓越的稳定性,单次转换效率高达 67%。通过原位拉曼分析,我们将这些性能提升归因于硅酸盐缓冲层的加入促进了二氧化碳的吸附和局部碱性环境。我们认为,添加缓冲层来调节微环境对于实现高性能和在酸性条件下保持稳定至关重要。
Enhanced electrochemical carbon dioxide reduction in membrane electrode assemblies with acidic electrolytes through a silicate buffer layer
The electrochemical reduction of CO2 holds considerable promise in combating global climate change while yielding valuable chemical commodities. Membrane electrode assemblies operating within acidic electrolyte have exhibited noteworthy advancements in CO2 utilization efficiency, albeit encountering formidable competition from the hydrogen evolution reaction. In our investigation, we introduced a silicate buffer layer, which yielded exceptional outcomes even using strong acid electrolyte. Notably, our approach yielded a CO Faradic efficiency of 90% and reached a substantial current density of 400 mA cm–2. Furthermore, our system displayed remarkable stability over a 12-hour duration, and achieved a high single-pass-conversion efficiency of 67%. Leveraging in-situ Raman analysis, we attributed these performance enhancements to the augmented CO2 adsorption and localized alkaline environment facilitated by the incorporation of the silicate buffer layer. We think the addition of buffer layer to adjust the microenvironment is essential to achieve high performance and keep stable in acid condition.
期刊介绍:
The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.