Excitonic Au4Ru2(PPh3)2(SC2H4Ph)8 cluster for light-driven dinitrogen fixation

Yongnan Sun; Wei Pei; Mingcai Xie; Shun Xu; Si Zhou; Jijun Zhao; Kang Xiao; Yan Zhu

doi:10.1039/C9SC06424A

Excitonic Au₄Ru₂(PPh₃)₂(SC₂H₄Ph)₈ cluster for light-driven dinitrogen fixation†

Yongnan Sun,‡^a Wei Pei,‡^b Mingcai Xie,

^a Shun Xu,^a Si Zhou,

*^b Jijun Zhao,

^b Kang Xiao^c and Yan Zhu

*^a

Author affiliations

* Corresponding authors

^a Key Lab of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, China
E-mail: zhuyan@nju.edu.cn

^b Key Laboratory of Materials Modification by Laser, Ion and Electron Beams, Dalian University of Technology, Dalian 116024, China
E-mail: sizhou@dlut.edu.cn

^c School of Materials Science and Engineering, Nanjing University of Posts and Telecommunications, Nanjing 210023, China

Abstract

The surface plasmon resonance of metal nanoparticles has been widely used to improve photochemical transformations by plasmon-induced charge transfer. However, it remains elusive for the molecular-like metal clusters with non-metallic or excitonic behavior to enable light harvesting including electron/hole pair production and separation. Here we report a paradigm for solar energy conversion on an atomically precise Au₄Ru₂ cluster supported on TiO₂ with oxygen vacancies, in which the electron–hole pairs can be directly generated from the excited Au₄Ru₂ cluster and the TiO₂ support, and the photogenerated electrons can transfer to the Ru atoms. Importantly, the Ru atoms in the Au₄Ru₂ cluster are capable of injecting the electrons into adsorbed N₂ to activate N₂ molecules. The cooperative effect in the supported Au₄Ru₂ catalyst efficiently boosts the photocatalytic activity for N₂ fixation in comparison with homogold (Au_n) clusters.

This article is part of the themed collection: Celebrating a century of chemical excellence at Nanjing University

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Article information

DOI: https://doi.org/10.1039/C9SC06424A
Article type: Edge Article
Submitted: 19 Dec 2019
Accepted: 21 Jan 2020
First published: 27 Jan 2020
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry

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Chem. Sci., 2020,11, 2440-2447

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Excitonic Au₄Ru₂(PPh₃)₂(SC₂H₄Ph)₈ cluster for light-driven dinitrogen fixation

Y. Sun, W. Pei, M. Xie, S. Xu, S. Zhou, J. Zhao, K. Xiao and Y. Zhu, Chem. Sci., 2020, 11, 2440 DOI: 10.1039/C9SC06424A

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