Luhan Li, Zenan Li, Jiacheng Li, Jiaxuan Wang, Haojie Xu, Haizhou Yu, Qianyu Lin, Hui Huang, Yang Liu, Zhenhui Kang
{"title":"氨基酚修饰金纳米团簇在二步单电子氧还原反应中光合成H2O2的异构体效应","authors":"Luhan Li, Zenan Li, Jiacheng Li, Jiaxuan Wang, Haojie Xu, Haizhou Yu, Qianyu Lin, Hui Huang, Yang Liu, Zhenhui Kang","doi":"10.1002/smll.202410843","DOIUrl":null,"url":null,"abstract":"<p>Gold (Au) nanoclustersare promising photocatalysts for biomedicine, sensing, and environmental remediation. However, the short carrier lifetime, inherent instability, and unclear charge transfer mechanism hinder their application. Herein, the Au nanoclusters decorated with three different isomers of o-Aminophenol, m-Aminophenol, and p-Aminophenol are synthesized, namely o-Au, m-Au, and p-Au, which achieve efficient hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) photoproduction through two-step one-electron oxygen reduction reaction (ORR). The interfacial kinetics for the photocatalytic process in this system are investigated in detail, in which, the isomer-effects of aminophenol decorated in Au nanoclusters are definitely elucidated by combining transient photovoltage (TPV), transient potential scanning (TPS), and photo-induced current (TPC) tests. The reaction pathway of o-Au, m-Au, and p-Au is confirmed to be the same through TPC. Although the conduction band values of o-Au, m-Au, and p-Au are essentially the same under working conditions, the values of surface effective charges (n<sub>e</sub>) for both m-Au and p-Au are higher than that of o-Au. In addition, m-Au has a stronger adsorption capacity for O<sub>2</sub> and a faster ORR rate. Thus, the m-Au manifests the highest photocatalytic activity for the H<sub>2</sub>O<sub>2</sub> photoproduction. This work shows a new way for the <i>in</i><i>-</i><i>situ</i> study on charge distribution and transfer on photocatalysts.</p>","PeriodicalId":228,"journal":{"name":"Small","volume":"21 7","pages":""},"PeriodicalIF":12.1000,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Isomer-Effects of Aminophenol Decorated Gold Nanoclusters for H2O2 Photoproduction via Two-Step One-Electron Oxygen Reduction Reaction\",\"authors\":\"Luhan Li, Zenan Li, Jiacheng Li, Jiaxuan Wang, Haojie Xu, Haizhou Yu, Qianyu Lin, Hui Huang, Yang Liu, Zhenhui Kang\",\"doi\":\"10.1002/smll.202410843\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Gold (Au) nanoclustersare promising photocatalysts for biomedicine, sensing, and environmental remediation. However, the short carrier lifetime, inherent instability, and unclear charge transfer mechanism hinder their application. Herein, the Au nanoclusters decorated with three different isomers of o-Aminophenol, m-Aminophenol, and p-Aminophenol are synthesized, namely o-Au, m-Au, and p-Au, which achieve efficient hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) photoproduction through two-step one-electron oxygen reduction reaction (ORR). The interfacial kinetics for the photocatalytic process in this system are investigated in detail, in which, the isomer-effects of aminophenol decorated in Au nanoclusters are definitely elucidated by combining transient photovoltage (TPV), transient potential scanning (TPS), and photo-induced current (TPC) tests. The reaction pathway of o-Au, m-Au, and p-Au is confirmed to be the same through TPC. Although the conduction band values of o-Au, m-Au, and p-Au are essentially the same under working conditions, the values of surface effective charges (n<sub>e</sub>) for both m-Au and p-Au are higher than that of o-Au. In addition, m-Au has a stronger adsorption capacity for O<sub>2</sub> and a faster ORR rate. Thus, the m-Au manifests the highest photocatalytic activity for the H<sub>2</sub>O<sub>2</sub> photoproduction. This work shows a new way for the <i>in</i><i>-</i><i>situ</i> study on charge distribution and transfer on photocatalysts.</p>\",\"PeriodicalId\":228,\"journal\":{\"name\":\"Small\",\"volume\":\"21 7\",\"pages\":\"\"},\"PeriodicalIF\":12.1000,\"publicationDate\":\"2025-01-09\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Small\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/smll.202410843\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Small","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/smll.202410843","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Isomer-Effects of Aminophenol Decorated Gold Nanoclusters for H2O2 Photoproduction via Two-Step One-Electron Oxygen Reduction Reaction
Gold (Au) nanoclustersare promising photocatalysts for biomedicine, sensing, and environmental remediation. However, the short carrier lifetime, inherent instability, and unclear charge transfer mechanism hinder their application. Herein, the Au nanoclusters decorated with three different isomers of o-Aminophenol, m-Aminophenol, and p-Aminophenol are synthesized, namely o-Au, m-Au, and p-Au, which achieve efficient hydrogen peroxide (H2O2) photoproduction through two-step one-electron oxygen reduction reaction (ORR). The interfacial kinetics for the photocatalytic process in this system are investigated in detail, in which, the isomer-effects of aminophenol decorated in Au nanoclusters are definitely elucidated by combining transient photovoltage (TPV), transient potential scanning (TPS), and photo-induced current (TPC) tests. The reaction pathway of o-Au, m-Au, and p-Au is confirmed to be the same through TPC. Although the conduction band values of o-Au, m-Au, and p-Au are essentially the same under working conditions, the values of surface effective charges (ne) for both m-Au and p-Au are higher than that of o-Au. In addition, m-Au has a stronger adsorption capacity for O2 and a faster ORR rate. Thus, the m-Au manifests the highest photocatalytic activity for the H2O2 photoproduction. This work shows a new way for the in-situ study on charge distribution and transfer on photocatalysts.
期刊介绍:
Small serves as an exceptional platform for both experimental and theoretical studies in fundamental and applied interdisciplinary research at the nano- and microscale. The journal offers a compelling mix of peer-reviewed Research Articles, Reviews, Perspectives, and Comments.
With a remarkable 2022 Journal Impact Factor of 13.3 (Journal Citation Reports from Clarivate Analytics, 2023), Small remains among the top multidisciplinary journals, covering a wide range of topics at the interface of materials science, chemistry, physics, engineering, medicine, and biology.
Small's readership includes biochemists, biologists, biomedical scientists, chemists, engineers, information technologists, materials scientists, physicists, and theoreticians alike.