{"title":"利用活性氧构建电子富集 Ptδ+ 以增强丙烷催化燃烧","authors":"Zhixin Yu, Yarong Fang, Chuanqi Pan, Shiqi Ma, Yiqing Zeng, Ji Yang, Shipeng Wan, Zhaoxiang Zhong","doi":"10.1021/acsami.5c00598","DOIUrl":null,"url":null,"abstract":"The complete catalytic oxidation of propane (C<sub>3</sub>H<sub>8</sub>) at low temperatures remains challenging due to the competitive adsorption between the oxidation of the O<sub>2</sub> and C<sub>3</sub>H<sub>8</sub> molecules. In this study, we propose an innovative approach to enhance C<sub>3</sub>H<sub>8</sub> oxidation by strategically designing active Pt<sup>δ+</sup> sites with modulated electronic structures on F-doped TiO<sub>2</sub>-supported Pt catalyst (Pt/F-TiO<sub>2</sub>), which exhibits 50 and 90% of propane conversion at 200 and 320 °C. Our mechanistic study reveals that the electron coupling between Pt 5d and F 2p alters the d orbital electron property, which leads to generation of abundant efficient electron-enriched Pt<sup>δ+</sup> species. These new Pt<sup>δ+</sup> sites facilitate the adsorption of C<sub>3</sub>H<sub>8</sub> and promote the activation of chemisorbed O<sub>2</sub> into superoxide species, in the form of bridge Pt-(O–O)<sub>ad</sub>-Ti, which synergistically facilitates the methyl C–H cleavage in C<sub>3</sub>H<sub>8</sub>. This study presents the strategy for electronic structure engineering of active sites in Pt-based catalysts, paving the way for the development of high-performance catalysts for propane oxidation.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"24 1","pages":""},"PeriodicalIF":8.2000,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Construction of Electron-Enriched Ptδ+ with Reactive Oxygen Species for Enhanced Propane Catalytic Combustion\",\"authors\":\"Zhixin Yu, Yarong Fang, Chuanqi Pan, Shiqi Ma, Yiqing Zeng, Ji Yang, Shipeng Wan, Zhaoxiang Zhong\",\"doi\":\"10.1021/acsami.5c00598\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The complete catalytic oxidation of propane (C<sub>3</sub>H<sub>8</sub>) at low temperatures remains challenging due to the competitive adsorption between the oxidation of the O<sub>2</sub> and C<sub>3</sub>H<sub>8</sub> molecules. In this study, we propose an innovative approach to enhance C<sub>3</sub>H<sub>8</sub> oxidation by strategically designing active Pt<sup>δ+</sup> sites with modulated electronic structures on F-doped TiO<sub>2</sub>-supported Pt catalyst (Pt/F-TiO<sub>2</sub>), which exhibits 50 and 90% of propane conversion at 200 and 320 °C. Our mechanistic study reveals that the electron coupling between Pt 5d and F 2p alters the d orbital electron property, which leads to generation of abundant efficient electron-enriched Pt<sup>δ+</sup> species. These new Pt<sup>δ+</sup> sites facilitate the adsorption of C<sub>3</sub>H<sub>8</sub> and promote the activation of chemisorbed O<sub>2</sub> into superoxide species, in the form of bridge Pt-(O–O)<sub>ad</sub>-Ti, which synergistically facilitates the methyl C–H cleavage in C<sub>3</sub>H<sub>8</sub>. This study presents the strategy for electronic structure engineering of active sites in Pt-based catalysts, paving the way for the development of high-performance catalysts for propane oxidation.\",\"PeriodicalId\":5,\"journal\":{\"name\":\"ACS Applied Materials & Interfaces\",\"volume\":\"24 1\",\"pages\":\"\"},\"PeriodicalIF\":8.2000,\"publicationDate\":\"2025-03-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Materials & Interfaces\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acsami.5c00598\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Materials & Interfaces","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acsami.5c00598","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
Construction of Electron-Enriched Ptδ+ with Reactive Oxygen Species for Enhanced Propane Catalytic Combustion
The complete catalytic oxidation of propane (C3H8) at low temperatures remains challenging due to the competitive adsorption between the oxidation of the O2 and C3H8 molecules. In this study, we propose an innovative approach to enhance C3H8 oxidation by strategically designing active Ptδ+ sites with modulated electronic structures on F-doped TiO2-supported Pt catalyst (Pt/F-TiO2), which exhibits 50 and 90% of propane conversion at 200 and 320 °C. Our mechanistic study reveals that the electron coupling between Pt 5d and F 2p alters the d orbital electron property, which leads to generation of abundant efficient electron-enriched Ptδ+ species. These new Ptδ+ sites facilitate the adsorption of C3H8 and promote the activation of chemisorbed O2 into superoxide species, in the form of bridge Pt-(O–O)ad-Ti, which synergistically facilitates the methyl C–H cleavage in C3H8. This study presents the strategy for electronic structure engineering of active sites in Pt-based catalysts, paving the way for the development of high-performance catalysts for propane oxidation.
期刊介绍:
ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.