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

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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.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 22375020, 52272186, and 22105116) and Beijing Institute of Technology Research Fund Program for Young Scholars. We acknowledge the 1W1B station for XAFS measurement in the Beijing Synchrotron Radiation Facility (BSRF) and BL10B and BL12B in the National Synchrotron Radiation Laboratory (NSRL) for use of their instruments. We thank Analysis and Testing Center, Beijing Institute of Technology, for assistance in HRTEM and STEM-EDS experiments. We also thank Dr. Leining Zhang for her help on theoretical analysis.

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  1. 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

    Xiaoya Huang, Xinyuan Li, Akang Chen, Hongfei Gu, Shouyuan Li, Tailei Hou, Shuwen Zhu & Jiatao Zhang

  2. MIIT Key Laboratory of Complex-field Intelligent Exploration, School of Optics and Photonics, Beijing Institute of Technology, Beijing, 100081, China

    Shuang Yu & Yin Song

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  1. Xiaoya Huang
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Correspondence to Xinyuan Li or Jiatao Zhang.

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

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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 Res. (2024). https://doi.org/10.1007/s12274-024-6706-2

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