Zishuai Wang , Yaoqiang Wang , Gang Xiao , Yu Jin , Haijia Su
{"title":"Selective oxidation of polyols to primary hydroxyl acids by plasmonic catalysis on an Au–Pt nanoalloy irradiated by visible light†","authors":"Zishuai Wang , Yaoqiang Wang , Gang Xiao , Yu Jin , Haijia Su","doi":"10.1039/d5gc00299k","DOIUrl":null,"url":null,"abstract":"<div><div>The integration of plasmonic metals with active transition metal-based catalysts has the potential to expand the range of chemical reactions feasible through plasmonic photocatalysis. This study reports a photocatalyst combining plasmonic Au and catalytically active Pt in the form of an Au–Pt nanoalloy supported on ZrO<sub>2</sub> nanopowder. This photocatalyst operates more effectively and selectively for the oxidation of polyols under visible light illumination than under conventional conditions, demonstrating a promising green process. By meticulously contrasting the photoelectronic properties, optical absorption, and <em>in situ</em> characterization of the catalyst, we have been able to substantiate the synergistic and plasmonic effect that enhances reaction efficiency. Light-excited hot electrons were observed to enhance the adsorption of oxygen by the photocatalyst, thereby accelerating the formation of ˙O<sub>2</sub><sup>−</sup>. Intense electromagnetic near fields generated at the illuminated plasmonic photocatalyst were observed to significantly enhance the chemisorption of the reactant onto the catalyst surface and the desorption of products. This green photocatalytic procedure is effective in a continuous-flow reactor under ambient temperature, ambient pressure, and simulated sunlight irradiation, allowing for the gram-scale production of 0.58 g of glycolate from 0.62 g of ethylene glycol.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 13","pages":"Pages 3542-3550"},"PeriodicalIF":9.3000,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Green Chemistry","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/org/science/article/pii/S1463926225001530","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
Abstract
The integration of plasmonic metals with active transition metal-based catalysts has the potential to expand the range of chemical reactions feasible through plasmonic photocatalysis. This study reports a photocatalyst combining plasmonic Au and catalytically active Pt in the form of an Au–Pt nanoalloy supported on ZrO2 nanopowder. This photocatalyst operates more effectively and selectively for the oxidation of polyols under visible light illumination than under conventional conditions, demonstrating a promising green process. By meticulously contrasting the photoelectronic properties, optical absorption, and in situ characterization of the catalyst, we have been able to substantiate the synergistic and plasmonic effect that enhances reaction efficiency. Light-excited hot electrons were observed to enhance the adsorption of oxygen by the photocatalyst, thereby accelerating the formation of ˙O2−. Intense electromagnetic near fields generated at the illuminated plasmonic photocatalyst were observed to significantly enhance the chemisorption of the reactant onto the catalyst surface and the desorption of products. This green photocatalytic procedure is effective in a continuous-flow reactor under ambient temperature, ambient pressure, and simulated sunlight irradiation, allowing for the gram-scale production of 0.58 g of glycolate from 0.62 g of ethylene glycol.
期刊介绍:
Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.