{"title":"通过掺杂 Fe3+ 梯度,利用内置电场 CsPbBr3/SiO2 纳米复合材料高效、选择性地光催化氧化苯甲醇","authors":"Peng Zhang, Feiming Li, Shujuan Lin, Wen-Jie Chen, Dejian Chen","doi":"10.1016/j.cej.2024.156953","DOIUrl":null,"url":null,"abstract":"Lead halide perovskite nanocrystals (PNCs) have emerged as promising materials for photocatalysis due to their exceptional optoelectronic properties, yet achieving efficient charge separation and selective oxidation reactions remains a significant challenge. In this study, we report the synthesis of Fe<sup>3+</sup>-doped CsPbBr<sub>3</sub>/SiO<sub>2</sub> nanocomposites (Fe-PNCs/SNPs) with gradient energy levels, designed to enhance photocatalytic performance. Our results demonstrate that Fe<sup>3+</sup> doping introduces mid-gap states, promotes photoinduced charge separation, and generates reactive oxygen species (ROS) such as <img alt=\"radical dot\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/rad.gif\" style=\"vertical-align:middle\"/>O<sub>2</sub><sup>−</sup> and <img alt=\"radical dot\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/rad.gif\" style=\"vertical-align:middle\"/>OH radicals under sunlight-simulating light irradiation from a 300 W Xe arc lamp. The Fe<sub>20</sub>-PNCs/SNPs catalyst achieved over 99 % conversion of benzyl alcohol to benzaldehyde with high selectivity and stability in the ethanol under ambient conditions. Additionally, the catalyst exhibited excellent recyclability and broad substrate tolerance. These findings highlight the innovative design of gradient energy levels in perovskite nanocomposites, offering a new strategy for enhancing photocatalytic efficiency in selective organic transformations.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":null,"pages":null},"PeriodicalIF":13.3000,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Efficient and selective photocatalytic oxidation of benzylic alcohols with built-in electric field CsPbBr3/SiO2 nanocomposites through Fe3+ gradient doping\",\"authors\":\"Peng Zhang, Feiming Li, Shujuan Lin, Wen-Jie Chen, Dejian Chen\",\"doi\":\"10.1016/j.cej.2024.156953\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Lead halide perovskite nanocrystals (PNCs) have emerged as promising materials for photocatalysis due to their exceptional optoelectronic properties, yet achieving efficient charge separation and selective oxidation reactions remains a significant challenge. In this study, we report the synthesis of Fe<sup>3+</sup>-doped CsPbBr<sub>3</sub>/SiO<sub>2</sub> nanocomposites (Fe-PNCs/SNPs) with gradient energy levels, designed to enhance photocatalytic performance. Our results demonstrate that Fe<sup>3+</sup> doping introduces mid-gap states, promotes photoinduced charge separation, and generates reactive oxygen species (ROS) such as <img alt=\\\"radical dot\\\" src=\\\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/rad.gif\\\" style=\\\"vertical-align:middle\\\"/>O<sub>2</sub><sup>−</sup> and <img alt=\\\"radical dot\\\" src=\\\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/rad.gif\\\" style=\\\"vertical-align:middle\\\"/>OH radicals under sunlight-simulating light irradiation from a 300 W Xe arc lamp. The Fe<sub>20</sub>-PNCs/SNPs catalyst achieved over 99 % conversion of benzyl alcohol to benzaldehyde with high selectivity and stability in the ethanol under ambient conditions. Additionally, the catalyst exhibited excellent recyclability and broad substrate tolerance. These findings highlight the innovative design of gradient energy levels in perovskite nanocomposites, offering a new strategy for enhancing photocatalytic efficiency in selective organic transformations.\",\"PeriodicalId\":270,\"journal\":{\"name\":\"Chemical Engineering Journal\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":13.3000,\"publicationDate\":\"2024-10-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Engineering Journal\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1016/j.cej.2024.156953\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.cej.2024.156953","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Efficient and selective photocatalytic oxidation of benzylic alcohols with built-in electric field CsPbBr3/SiO2 nanocomposites through Fe3+ gradient doping
Lead halide perovskite nanocrystals (PNCs) have emerged as promising materials for photocatalysis due to their exceptional optoelectronic properties, yet achieving efficient charge separation and selective oxidation reactions remains a significant challenge. In this study, we report the synthesis of Fe3+-doped CsPbBr3/SiO2 nanocomposites (Fe-PNCs/SNPs) with gradient energy levels, designed to enhance photocatalytic performance. Our results demonstrate that Fe3+ doping introduces mid-gap states, promotes photoinduced charge separation, and generates reactive oxygen species (ROS) such as O2− and OH radicals under sunlight-simulating light irradiation from a 300 W Xe arc lamp. The Fe20-PNCs/SNPs catalyst achieved over 99 % conversion of benzyl alcohol to benzaldehyde with high selectivity and stability in the ethanol under ambient conditions. Additionally, the catalyst exhibited excellent recyclability and broad substrate tolerance. These findings highlight the innovative design of gradient energy levels in perovskite nanocomposites, offering a new strategy for enhancing photocatalytic efficiency in selective organic transformations.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.