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基于天线-反应体系肖特基结的表面等离激元驱动热电子的催化增强。

Catalytic Boosting by Surface-Plasmon-Driven Hot Electrons on Antenna-Reactor Schottky Nanodiodes.

机构信息

Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701, Republic of Korea.

出版信息

Nano Lett. 2023 Jun 14;23(11):5116-5122. doi: 10.1021/acs.nanolett.3c01037. Epub 2023 Jun 2.

Abstract

Significant research has focused on enhancing catalytic performance through solar energy conversion, and the design of photocatalysis incorporating surface plasmons is drawing considerable attention as a highly competitive catalyst system. Although the hot electron process is the primary mechanism in plasmonic photocatalysis, the precise function of hot electron transport in catalytic reactions remains unclear due to the absence of direct measurement. Here, we demonstrate the intrinsic relationship between surface-plasmon-driven hot electrons and catalytic activity during hydrogen oxidation, utilizing catalytic Schottky nanodiodes (Pt/Ag/TiO) for antenna-reactor plasmonic photocatalysis. The simultaneous and independent measurements of hot electron flow and catalytic turnover rate show that the plasmonic effect amplifies the flow of reaction-induced hot electrons (chemicurrent), leading to enhanced catalytic activity. Plasmonic photocatalytic performance can be controlled with light wavelengths, intensity, surface temperature, and structures. These results elucidate the hot electron flow on photocatalysis and offer improved strategies for efficient catalytic devices.

摘要

大量研究集中在通过太阳能转换来提高催化性能,而将表面等离激元纳入光催化设计作为一种极具竞争力的催化剂系统正引起广泛关注。尽管在等离子体光催化中,热电子过程是主要机制,但由于缺乏直接测量,热电子输运在催化反应中的精确功能仍不清楚。在这里,我们利用天线-反应器等离子体光催化中的肖特基纳米二极管(Pt/Ag/TiO),展示了表面等离激元驱动的热电子与氧化氢过程中催化活性之间的内在关系。热电子流和催化周转率的同时独立测量表明,等离激元效应放大了反应诱导的热电子(化学电流)的流动,从而提高了催化活性。可以用光的波长、强度、表面温度和结构来控制等离子体光催化性能。这些结果阐明了光催化中的热电子流动,并为高效催化器件提供了改进的策略。

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