活性位点的分离和电子传递的增强促进了多功能金属有机框架的光催化二氧化碳还原作用

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL
Zitong Wang, Pierce Yeary, Yingjie Fan, Chenghua Deng and Wenbin Lin*, 
{"title":"活性位点的分离和电子传递的增强促进了多功能金属有机框架的光催化二氧化碳还原作用","authors":"Zitong Wang,&nbsp;Pierce Yeary,&nbsp;Yingjie Fan,&nbsp;Chenghua Deng and Wenbin Lin*,&nbsp;","doi":"10.1021/acscatal.4c02326","DOIUrl":null,"url":null,"abstract":"<p >We report a multifunctional metal–organic framework (MOF) photocatalyst for the CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) under visible light irradiation with high efficiency (turnover number = 2638) and CO selectivity (97.0%). The short distance (6.6 Å) between bipyridine sites in the MOF allows the integration of Ir photosensitizers and Ni catalysts in proximity, thereby enhancing their electron transfer for photocatalytic CO<sub>2</sub>RR. Isolation of these metal centers by the MOF structure prevents their deactivation, leading to 54 times higher CO<sub>2</sub>RR activity than the homogeneous system and allowing for easy recovery for use in five consecutive cycles of photocatalytic CO<sub>2</sub>RR without significant loss of catalytic activity.</p>","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"14 12","pages":"9217–9223"},"PeriodicalIF":13.1000,"publicationDate":"2024-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Active Site Isolation and Enhanced Electron Transfer Facilitate Photocatalytic CO2 Reduction by A Multifunctional Metal–Organic Framework\",\"authors\":\"Zitong Wang,&nbsp;Pierce Yeary,&nbsp;Yingjie Fan,&nbsp;Chenghua Deng and Wenbin Lin*,&nbsp;\",\"doi\":\"10.1021/acscatal.4c02326\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >We report a multifunctional metal–organic framework (MOF) photocatalyst for the CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) under visible light irradiation with high efficiency (turnover number = 2638) and CO selectivity (97.0%). The short distance (6.6 Å) between bipyridine sites in the MOF allows the integration of Ir photosensitizers and Ni catalysts in proximity, thereby enhancing their electron transfer for photocatalytic CO<sub>2</sub>RR. Isolation of these metal centers by the MOF structure prevents their deactivation, leading to 54 times higher CO<sub>2</sub>RR activity than the homogeneous system and allowing for easy recovery for use in five consecutive cycles of photocatalytic CO<sub>2</sub>RR without significant loss of catalytic activity.</p>\",\"PeriodicalId\":9,\"journal\":{\"name\":\"ACS Catalysis \",\"volume\":\"14 12\",\"pages\":\"9217–9223\"},\"PeriodicalIF\":13.1000,\"publicationDate\":\"2024-06-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Catalysis \",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acscatal.4c02326\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acscatal.4c02326","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

摘要

我们报告了一种多功能金属有机框架(MOF)光催化剂,该催化剂可在可见光照射下进行二氧化碳还原反应(CO2RR),具有高效率(转化率 = 2638)和二氧化碳选择性(97.0%)。MOF 中的双吡啶位点之间的距离很短(6.6 Å),因此可以将 Ir 光敏剂和 Ni 催化剂整合在一起,从而增强它们在光催化 CO2RR 反应中的电子传递。MOF 结构隔离了这些金属中心,防止了它们的失活,从而使 CO2RR 活性比均相体系高出 54 倍,并可在光催化 CO2RR 的连续五个循环中轻松恢复使用,而不会明显丧失催化活性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Active Site Isolation and Enhanced Electron Transfer Facilitate Photocatalytic CO2 Reduction by A Multifunctional Metal–Organic Framework

Active Site Isolation and Enhanced Electron Transfer Facilitate Photocatalytic CO2 Reduction by A Multifunctional Metal–Organic Framework

Active Site Isolation and Enhanced Electron Transfer Facilitate Photocatalytic CO2 Reduction by A Multifunctional Metal–Organic Framework

We report a multifunctional metal–organic framework (MOF) photocatalyst for the CO2 reduction reaction (CO2RR) under visible light irradiation with high efficiency (turnover number = 2638) and CO selectivity (97.0%). The short distance (6.6 Å) between bipyridine sites in the MOF allows the integration of Ir photosensitizers and Ni catalysts in proximity, thereby enhancing their electron transfer for photocatalytic CO2RR. Isolation of these metal centers by the MOF structure prevents their deactivation, leading to 54 times higher CO2RR activity than the homogeneous system and allowing for easy recovery for use in five consecutive cycles of photocatalytic CO2RR without significant loss of catalytic activity.

求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信