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等离子体激元促进的原子间热载流子调控增强电催化氮还原反应

Plasmon-Promoted Interatomic Hot Carriers Regulation Enhanced Electrocatalytic Nitrogen Reduction Reaction.

作者信息

Liang Wenkai, Xie Miao, Li Dong, Qin Wei, Dai Chang, Wang Yawen, Zhang Hao, Zhao Bo, Jin Guangyao, Sun Yinghui, Jiang Lin

机构信息

Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, 215123, Suzhou, China.

Nonequilibrium Chemical Physics, TUM School of Natural Sciences, Technical University of Munich, 85748, Garching, Germany.

出版信息

Angew Chem Int Ed Engl. 2024 Nov 25;63(48):e202409484. doi: 10.1002/anie.202409484. Epub 2024 Oct 24.

Abstract

Utilizing hot carriers for efficient plasmon-mediated chemical reactions (PMCRs) to convert solar energy into secondary energy is one of the most feasible solutions to the global environmental and energy crisis. Finding a plasmonic heterogeneous nanostructure with a more efficient and reasonable hot carrier transport path without affecting the intrinsic plasmonic properties is still a major challenge that urgently needs to be solved in this field. Herein, the mechanism by which plasmon-promoted interatomic hot electron redistribution on the surface of AuCu alloy nanoparticles promotes the electrocatalytic nitrogen reduction reaction (ENRR) is successfully clarified. The localized surface plasmon resonance (LSPR) effect can boost the transfer of plasmon hot electrons from Au atoms to Cu atoms, trigger the interatomic electron regulation of AuCu alloy nanoparticles, enhance the desorption of ammonia molecules, and increase the ammonia yield by approximately 93.9 %. This work provides an important reference for rationally designing and utilizing the LSPR effect to efficiently regulate the distribution and mechanism of plasmon hot carriers on the surface of heterogeneous alloy nanostructures.

摘要

利用热载流子实现高效的等离子体介导化学反应(PMCRs),将太阳能转化为二次能源,是解决全球环境和能源危机最可行的方案之一。在不影响固有等离子体特性的情况下,找到一种具有更高效、合理热载流子传输路径的等离子体异质纳米结构,仍然是该领域迫切需要解决的一个主要挑战。在此,成功阐明了等离子体促进金铜合金纳米颗粒表面原子间热电子重新分布促进电催化氮还原反应(ENRR)的机制。局域表面等离子体共振(LSPR)效应可促进等离子体热电子从金原子向铜原子的转移,触发金铜合金纳米颗粒的原子间电子调控,增强氨分子的解吸,并使氨产量提高约93.9%。这项工作为合理设计和利用LSPR效应以有效调节异质合金纳米结构表面等离子体热载流子的分布和机制提供了重要参考。

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