利用溴化物官能化聚氧金属铝酸盐首次光催化合成二氧化碳环碳酸盐，无需额外的催化剂

IF 7.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Sustainable Chemistry & Engineering Pub Date : 2024-10-23 DOI:10.1021/acssuschemeng.4c06676

Huafeng Li, Hui Kong, Jianzhong Guo, Bing Li, Shanshan Zhang, Suzhi Li, Junwei Zhao, Liqun Bai

{"title":"利用溴化物官能化聚氧金属铝酸盐首次光催化合成二氧化碳环碳酸盐，无需额外的催化剂","authors":"Huafeng Li, Hui Kong, Jianzhong Guo, Bing Li, Shanshan Zhang, Suzhi Li, Junwei Zhao, Liqun Bai","doi":"10.1021/acssuschemeng.4c06676","DOIUrl":null,"url":null,"abstract":"Developing photocatalysts with low energy consumption and high efficiency for CO2 fixation without any cocatalyst is a highly sought-after goal, but it still presents a significant challenge. Herein, aiming at enhancing the efficiency of photodriven CO2 cycloaddition reactions, an imidazolium bromide ionic liquid-functionalized polyoxometalate photocatalyst ImBr-[Ru(C10N2H8)2]H[AsW12O40]·2H2O with Ru-based photosensitizer coordinated with ionic liquids via strong coupling between the metal active site and carboxy group is reported. The optimized ImBr-[Ru(C10N2H8)2]H[AsW12O40]·2H2O achieves efficient photocatalytic CO2 cycloaddition with epoxides at ambient temperature without additional cocatalyst and photosensitizer, which is much higher than most reported photocatalysts in the presence of TBAB cocatalyst. The experimental results indicated that imidazolium bromide ionic liquid facilitating the ring-opened reaction of epoxides, the radical mechanism, and a plausible reaction pathway for the epoxidation step was further proposed by in situ DRIFT and EPR. Remarkably, this is the first report on the photoeffect of polyoxometalate-based catalysts with ionic liquid-functionalized molecules for catalytic CO2 photofixation without any cocatalyst and sacrificial agent.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"93 1","pages":""},"PeriodicalIF":7.3000,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"First Photocatalytic Synthesis of Cyclic Carbonates from CO2 Using Bromide-Functionalized Polyoxometalate without Additional Cocatalyst\",\"authors\":\"Huafeng Li, Hui Kong, Jianzhong Guo, Bing Li, Shanshan Zhang, Suzhi Li, Junwei Zhao, Liqun Bai\",\"doi\":\"10.1021/acssuschemeng.4c06676\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Developing photocatalysts with low energy consumption and high efficiency for CO2 fixation without any cocatalyst is a highly sought-after goal, but it still presents a significant challenge. Herein, aiming at enhancing the efficiency of photodriven CO2 cycloaddition reactions, an imidazolium bromide ionic liquid-functionalized polyoxometalate photocatalyst ImBr-[Ru(C10N2H8)2]H[AsW12O40]·2H2O with Ru-based photosensitizer coordinated with ionic liquids via strong coupling between the metal active site and carboxy group is reported. The optimized ImBr-[Ru(C10N2H8)2]H[AsW12O40]·2H2O achieves efficient photocatalytic CO2 cycloaddition with epoxides at ambient temperature without additional cocatalyst and photosensitizer, which is much higher than most reported photocatalysts in the presence of TBAB cocatalyst. The experimental results indicated that imidazolium bromide ionic liquid facilitating the ring-opened reaction of epoxides, the radical mechanism, and a plausible reaction pathway for the epoxidation step was further proposed by in situ DRIFT and EPR. Remarkably, this is the first report on the photoeffect of polyoxometalate-based catalysts with ionic liquid-functionalized molecules for catalytic CO2 photofixation without any cocatalyst and sacrificial agent.\",\"PeriodicalId\":25,\"journal\":{\"name\":\"ACS Sustainable Chemistry & Engineering\",\"volume\":\"93 1\",\"pages\":\"\"},\"PeriodicalIF\":7.3000,\"publicationDate\":\"2024-10-23\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Sustainable Chemistry & Engineering\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acssuschemeng.4c06676\",\"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":"ACS Sustainable Chemistry & Engineering","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acssuschemeng.4c06676","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

摘要

开发低能耗、高效率的光催化剂，在不使用任何助催化剂的情况下固定二氧化碳是人们孜孜以求的目标，但这仍然是一个巨大的挑战。本文以提高光驱动 CO2 环加成反应的效率为目标，报道了一种咪唑溴离子液体功能化聚氧化金属酸盐光催化剂 ImBr-[Ru(C10N2H8)2]H[AsW12O40]-2H2O，其 Ru 基光敏剂通过金属活性位点和羧基之间的强耦合与离子液体配位。优化后的 ImBr-[Ru(C10N2H8)2]H[AsW12O40]-2H2O不需要额外的助催化剂和光敏剂，就能在常温下高效光催化 CO2 与环氧化物的环加成反应，其效率远高于大多数已报道的在 TBAB 助催化剂存在下的光催化剂。实验结果表明，溴化咪唑离子液体促进了环氧化物的开环反应、自由基机理，并通过原位 DRIFT 和 EPR 进一步提出了环氧化步骤的合理反应途径。值得注意的是，这是首次报道在不使用任何共催化剂和牺牲剂的情况下，使用离子液体官能化分子的聚氧化金属催化剂催化二氧化碳光固化的光效应。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

First Photocatalytic Synthesis of Cyclic Carbonates from CO2 Using Bromide-Functionalized Polyoxometalate without Additional Cocatalyst

查看原文本刊更多论文

First Photocatalytic Synthesis of Cyclic Carbonates from CO2 Using Bromide-Functionalized Polyoxometalate without Additional Cocatalyst

Developing photocatalysts with low energy consumption and high efficiency for CO₂ fixation without any cocatalyst is a highly sought-after goal, but it still presents a significant challenge. Herein, aiming at enhancing the efficiency of photodriven CO₂ cycloaddition reactions, an imidazolium bromide ionic liquid-functionalized polyoxometalate photocatalyst ImBr-[Ru(C₁₀N₂H₈)₂]H[AsW₁₂O₄₀]·2H₂O with Ru-based photosensitizer coordinated with ionic liquids via strong coupling between the metal active site and carboxy group is reported. The optimized ImBr-[Ru(C₁₀N₂H₈)₂]H[AsW₁₂O₄₀]·2H₂O achieves efficient photocatalytic CO₂ cycloaddition with epoxides at ambient temperature without additional cocatalyst and photosensitizer, which is much higher than most reported photocatalysts in the presence of TBAB cocatalyst. The experimental results indicated that imidazolium bromide ionic liquid facilitating the ring-opened reaction of epoxides, the radical mechanism, and a plausible reaction pathway for the epoxidation step was further proposed by in situ DRIFT and EPR. Remarkably, this is the first report on the photoeffect of polyoxometalate-based catalysts with ionic liquid-functionalized molecules for catalytic CO₂ photofixation without any cocatalyst and sacrificial agent.

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 Sustainable Chemistry & Engineering CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL

CiteScore

13.80

自引率

4.80%

发文量

1470

审稿时长

1.7 months

期刊介绍： ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment. The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.