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Research Article

Electronic structure engineering of single atomic sites by plasmon-induced hot electrons for highly efficient and selective photocatalysis

Xiaoya Huang1, Xinyuan Li1( ), Akang Chen1, Hongfei Gu1, Shouyuan Li1, Tailei Hou1, Shuwen Zhu1, Shuang Yu2, Yin Song2, Jiatao Zhang1( )
Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, MIIT Key Laboratory of Medical Molecule Science and Pharmaceutical Engineering, MOE Key Laboratory of Cluster Science, School of Chemistry and Chemical Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
MIIT Key Laboratory of Complex-field Intelligent Exploration, School of Optics and Photonics, Beijing Institute of Technology, Beijing 100081, China
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Graphical Abstract

Localized surface plasmon resonance (LSPR) modulates the localized electronic structures of single atomic sites, thereby exhibiting high selectivity and high reduction activity for CO2RR with H2O under visible light irradiation.

Abstract

Single atom (SA) catalysts have achieved great success on highly selective heterogeneous catalysis due to their abundant and homogeneous active sites. The electronic structures of these active sites, restrained by their localized coordination environments, significantly determine their catalytic performances, which are difficult to manipulate. Here, we investigated the effect of localized surface plasmon resonance (LSPR) on engineering the electronic structures of single atomic sites. Typically, core–shell structures consisted of Au core and transition metal SAs loaded N-doped carbon (CN) shell were constructed, namely Au@M-SA/CN (M = Ni, Fe, and Co). It was demonstrated that plasmon-induced hot electrons originated from Au were directionally injected to the M-SAs under visible light irradiation, which significantly changed their electronic structures and meanwhile facilitated improved overall charge separation efficiency. The as-prepared Au@Ni-SA/CN exhibited highly efficient and selective photocatalytic CO2 reduction to CO performance, which is 20.8, 17.5, and 6.9 times those of Au nanoparticles, Au@CN, and Ni-SA/CN, respectively. Complementary spectroscopy analysis and theoretical calculations confirmed that the plasmon enhanced Ni-SA/CN sites featured increased charge density for efficient intermediate activation, contributing to the superb photocatalytic performance. The work provides a new insight on plasmon and atomic site engineering for efficient and selective catalysis.

Keywords

single atom catalystsplasmon enhancementcoupling effectphotocatalysisCO2 reduction

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Nano Research
Volume 17 Issue 8,
August 2024
Pages 6960-6967
DOI: 10.1007/s12274-024-6706-2
Cite this article:
Huang X, Li X, Chen A, et al. Electronic structure engineering of single atomic sites by plasmon-induced hot electrons for highly efficient and selective photocatalysis. Nano Research, 2024, 17(8): 6960-6967. https://doi.org/10.1007/s12274-024-6706-2
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Received: 03 March 2024
Revised: 12 April 2024
Accepted: 15 April 2024
Published: 18 May 2024
© Tsinghua University Press 2024
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