Infrared Light-Induced Anomalous Defect-Mediated Plasmonic Hot Electron Transfer for Enhanced Photocatalytic Hydrogen Evolution

Zichao Lian; Fan Wu; Jiangzhi Zi; Guisheng Li; Wei Wang; Hexing Li

doi:10.1021/jacs.3c03990

Infrared Light-Induced Anomalous Defect-Mediated Plasmonic Hot Electron Transfer for Enhanced Photocatalytic Hydrogen Evolution

J Am Chem Soc. 2023 Jul 19;145(28):15482-15487. doi: 10.1021/jacs.3c03990. Epub 2023 Jul 7.

Authors

Zichao Lian¹, Fan Wu¹, Jiangzhi Zi¹, Guisheng Li¹, Wei Wang^{2

3}, Hexing Li¹

Affiliations

¹ School of Materials and Chemistry, University of Shanghai for Science and Technology, Shanghai 200093, P. R. China.
² Department of Pharmacology and Toxicology, University of Arizona, Tucson, Arizona 85721, United States.
³ Department of Chemistry and Biochemistry, University of Arizona, Tucson, Arizona 85721, United States.

PMID: 37418381
DOI: 10.1021/jacs.3c03990

Abstract

Efficient utilization of infrared (IR) light, which occupies almost half of the solar energy, is an important but challenging task in solar-to-fuel transformation. Herein, we report the discovery of CuS@ZnS core@shell nanocrystals (CSNCs) with strong localized surface plasmon resonance (LSPR) characteristics in the IR light region showing enhanced photocatalytic activity in hydrogen evolution reaction (HER). A unique "plasmon-induced defect-mediated carrier transfer" (PIDCT) at the heterointerfaces of the CSNCs divulged by time-resolved transient spectroscopy enables producing a high quantum yield of 29.2%. The CuS@ZnS CSNCs exhibit high activity and stability in H₂ evolution under near-IR light irradiation. The HER rate of CuS@ZnS CSNCs at 26.9 μmol h^-1 g^-1 is significantly higher than those of CuS NCs (0.4 μmol h^-1 g^-1) and CuS/ZnS core/satellite heterostructured NCs (15.6 μmol h^-1 g^-1). The PIDCT may provide a viable strategy for the tuning of LSPR-generated carrier kinetics through controlling the defect engineering to improve photocatalytic performance.