{"title":"封闭在共价聚合物网络中的分子自组装光电催化二氧化碳还原成甲醇。","authors":"Yanjie Fang, Yifan Gao, Yingke Wen, Xinjia He, Thomas J Meyer, Bing Shan","doi":"10.1021/jacs.4c07949","DOIUrl":null,"url":null,"abstract":"<p><p>Inspired by the porous structures of photosynthetic organelles, we report here a new type of photoelectrode based on a standalone macroporous conjugated polymer network (MCN) that converts sunlight into high-energy electrons for CO<sub>2</sub> reduction to CH<sub>3</sub>OH. The MCN provides supramolecular cavities with sufficient functional groups that control the structures of photocatalytic assemblies, which circumvents the geometric limitations of traditional inorganic counterparts. Stabilized interfacial contact between MCN and photocatalysts is achieved by strong chemical linkages throughout the network. Solar irradiation of MCN with a cobalt-based catalyst generates highly reducing electrons for the reduction of CO<sub>2</sub> to CH<sub>3</sub>OH at a conversion efficiency of 70%. Production of CH<sub>3</sub>OH sustains for at least 100 h, with a small decrease in yield rates. Scaling up the photoelectrode from 1 to 100 cm<sup>2</sup> results in photocurrent generation stabilized at 0.25 A and continuous CH<sub>3</sub>OH production at a conversion efficiency of 85%, demonstrating the scalability and high performances.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":null,"pages":null},"PeriodicalIF":14.4000,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Photoelectrocatalytic CO<sub>2</sub> Reduction to Methanol by Molecular Self-Assemblies Confined in Covalent Polymer Networks.\",\"authors\":\"Yanjie Fang, Yifan Gao, Yingke Wen, Xinjia He, Thomas J Meyer, Bing Shan\",\"doi\":\"10.1021/jacs.4c07949\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Inspired by the porous structures of photosynthetic organelles, we report here a new type of photoelectrode based on a standalone macroporous conjugated polymer network (MCN) that converts sunlight into high-energy electrons for CO<sub>2</sub> reduction to CH<sub>3</sub>OH. The MCN provides supramolecular cavities with sufficient functional groups that control the structures of photocatalytic assemblies, which circumvents the geometric limitations of traditional inorganic counterparts. Stabilized interfacial contact between MCN and photocatalysts is achieved by strong chemical linkages throughout the network. Solar irradiation of MCN with a cobalt-based catalyst generates highly reducing electrons for the reduction of CO<sub>2</sub> to CH<sub>3</sub>OH at a conversion efficiency of 70%. Production of CH<sub>3</sub>OH sustains for at least 100 h, with a small decrease in yield rates. Scaling up the photoelectrode from 1 to 100 cm<sup>2</sup> results in photocurrent generation stabilized at 0.25 A and continuous CH<sub>3</sub>OH production at a conversion efficiency of 85%, demonstrating the scalability and high performances.</p>\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":14.4000,\"publicationDate\":\"2024-08-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Chemical Society\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/jacs.4c07949\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.4c07949","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Photoelectrocatalytic CO2 Reduction to Methanol by Molecular Self-Assemblies Confined in Covalent Polymer Networks.
Inspired by the porous structures of photosynthetic organelles, we report here a new type of photoelectrode based on a standalone macroporous conjugated polymer network (MCN) that converts sunlight into high-energy electrons for CO2 reduction to CH3OH. The MCN provides supramolecular cavities with sufficient functional groups that control the structures of photocatalytic assemblies, which circumvents the geometric limitations of traditional inorganic counterparts. Stabilized interfacial contact between MCN and photocatalysts is achieved by strong chemical linkages throughout the network. Solar irradiation of MCN with a cobalt-based catalyst generates highly reducing electrons for the reduction of CO2 to CH3OH at a conversion efficiency of 70%. Production of CH3OH sustains for at least 100 h, with a small decrease in yield rates. Scaling up the photoelectrode from 1 to 100 cm2 results in photocurrent generation stabilized at 0.25 A and continuous CH3OH production at a conversion efficiency of 85%, demonstrating the scalability and high performances.
期刊介绍:
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