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

IF 12.1 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Small Pub Date : 2025-01-09 DOI:10.1002/smll.202410843
Luhan Li, Zenan Li, Jiacheng Li, Jiaxuan Wang, Haojie Xu, Haizhou Yu, Qianyu Lin, Hui Huang, Yang Liu, Zhenhui Kang
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引用次数: 0

摘要

金(Au)纳米团簇在生物医学、传感和环境修复等领域具有广阔的应用前景。然而,载流子寿命短、固有不稳定性和电荷转移机制不明确等问题阻碍了它们的应用。本文合成了以邻氨基酚、间氨基酚和对氨基酚三种不同异构体装饰的Au纳米团簇,即o-Au、m-Au和p-Au,通过两步单电子氧还原反应(ORR)实现了高效的过氧化氢(H2O2)光合成。详细研究了该体系光催化过程的界面动力学,并结合瞬态光电压(TPV)、瞬态电位扫描(TPS)和光感应电流(TPC)测试,明确地阐明了修饰氨基苯酚在金纳米团簇中的异构体效应。通过TPC验证了o-Au、m-Au和p-Au的反应途径是相同的。虽然在工作条件下o-Au、m-Au和p-Au的导带值基本相同,但m-Au和p-Au的表面有效电荷(ne)值均高于o-Au。此外,m-Au对O2具有更强的吸附能力和更快的ORR速率。因此,m-Au对H2O2的光催化活性最高。这项工作为光催化剂上电荷分布和转移的原位研究开辟了一条新的途径。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Isomer-Effects of Aminophenol Decorated Gold Nanoclusters for H2O2 Photoproduction via Two-Step One-Electron Oxygen Reduction Reaction

Isomer-Effects of Aminophenol Decorated Gold Nanoclusters for H2O2 Photoproduction via Two-Step One-Electron Oxygen Reduction Reaction

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.

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来源期刊
Small
Small 工程技术-材料科学:综合
CiteScore
17.70
自引率
3.80%
发文量
1830
审稿时长
2.1 months
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.
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