Xiangjiao Gong, Wenkai Teng, Wei Liu, Hang Xiao, He Li, Honghui Ou, Guidong Yang
{"title":"A Sucker-Reactor Polyoxometalate Assembled Superstructures for Efficient Photocatalytic Nitrogen Fixation","authors":"Xiangjiao Gong, Wenkai Teng, Wei Liu, Hang Xiao, He Li, Honghui Ou, Guidong Yang","doi":"10.1002/adma.202412924","DOIUrl":null,"url":null,"abstract":"<p>Designing a reaction system that integrates reactant capture and transformation in an artificial photosynthesis system to achieve high reaction efficiency remains challenging. Here, an ionic liquid (IL) -polyoxometalate (POM) superstructure photocatalyst (P2HPMo) is reported, where the anisotropy of the superstructure is allowed by adjusting the alkyl chain lengths of ILs. Experimental data and theoretical simulation show that ILs and POM serve as the “sucker” and “reactor” of the reaction system to capture and transform the reactants, respectively. In particular, the addition of quaternary phosphorous IL cations is not only conducive to the adsorption of N<sub>2</sub> but also effectively promotes the activation of N<sub>2</sub> by manipulating the energy band and electronic structure. Consequently, the synthesized P2HPMo exhibits an ammonia synthesis rate of 98 µmol·g<sub>cat</sub><sup>−1</sup>·h<sup>−1</sup>, which is one of the highest values available in a sacrificial agent-free system.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"37 3","pages":""},"PeriodicalIF":27.4000,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/adma.202412924","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Designing a reaction system that integrates reactant capture and transformation in an artificial photosynthesis system to achieve high reaction efficiency remains challenging. Here, an ionic liquid (IL) -polyoxometalate (POM) superstructure photocatalyst (P2HPMo) is reported, where the anisotropy of the superstructure is allowed by adjusting the alkyl chain lengths of ILs. Experimental data and theoretical simulation show that ILs and POM serve as the “sucker” and “reactor” of the reaction system to capture and transform the reactants, respectively. In particular, the addition of quaternary phosphorous IL cations is not only conducive to the adsorption of N2 but also effectively promotes the activation of N2 by manipulating the energy band and electronic structure. Consequently, the synthesized P2HPMo exhibits an ammonia synthesis rate of 98 µmol·gcat−1·h−1, which is one of the highest values available in a sacrificial agent-free system.
期刊介绍:
Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.