Synergizing plasmonic Au nanocages with 2D MoS 2 nanosheets for significant enhancement in photocatalytic hydrogen evolution

Peng, Rui; Ma, Xiaohan; Hood, Zachary D.; Boulesbaa, Abdelaziz; Puretzky, Alexander A.; Tong, Jianhua; Wu, Zili

doi:10.1039/D3TA01657A

Title: Synergizing plasmonic Au nanocages with 2D MoS ₂ nanosheets for significant enhancement in photocatalytic hydrogen evolution

Journal Article · Tue Aug 08 00:00:00 EDT 2023 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/D3TA01657A· OSTI ID:1992149

Peng, Rui ^[1];

^[2]; Hood, Zachary D. ^[3];

^[4]; Puretzky, Alexander A. ^[1];

^[5];

^[1]

Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA, Department of Materials Science and Engineering, Clemson University, Clemson, South Carolina 29634, USA
Applied Materials Division, Argonne National Laboratory, 9700 S. Cass Avenue, Lemont, Illinois 60439, USA
Department of Chemistry and Biochemistry, California State University Northridge, Northridge, California 91330, USA
Department of Materials Science and Engineering, Clemson University, Clemson, South Carolina 29634, USA

Plasmonic enhancement of photocatalytic hydrogen evolution has been achieved under visible light illumination by integrating strongly plasmonic metal particles such as gold (Au) with semiconducting materials. To understand the effect of plasmon resonance on the photocatalytic hydrogen evolution reaction (HER), in this work, we study the hydrogen evolution reaction (HER) over Au nanocages with systematically tunable localized surface plasmon resonance (LSPR) properties dispersed on an Al₂O₃ support and covered with multiphasic 2D MoS₂ nanosheets. It is interesting to observe that by tuning the LSPR wavelength of Au nanocages, an optimal enhancement in the photocatalytic HER can be obtained over the multiphasic 2D MoS₂ nanosheets. In particular, when the LSPR wavelength of Au nanocages is close to the absorption edge of MoS₂ nanosheets, a 40-fold increase is observed in the HER rate regarding bare MoS₂. Time-resolved transient absorption spectroscopy was conducted to explicitly identify the mechanisms behind the Au/MoS₂ system. The results suggest that near field enhancement (NFE) is the dominant LSPR process in this system and a detailed explanation of the working mechanism in this system is proposed. Governed by the NFE process, the energy of the surface plasma is transferred from Au nanocages to MoS₂ nanosheets to promote electron–hole excitation in MoS2, and the efficiency reaches the maximum when the LSPR wavelength of Au nanocages matches the MoS₂ light absorption edge, resulting in a significantly enhanced photocatalytic hydrogen yield compared to the bare MoS₂ nanosheets and Au/MoS₂ systems where the LSPR wavelengths of Au nanocages and MoS₂ nanosheet absorption edge do not match. The learning from this work provides insights into the design of highly efficient photocatalysts based on plasmonic materials.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725

OSTI ID:: 1992149

Alternate ID(s):: OSTI ID: 1994626

Journal Information:: Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Vol. 11 Journal Issue: 31; ISSN 2050-7488

Publisher:: Royal Society of Chemistry (RSC)Copyright Statement

Country of Publication:: United Kingdom

Language:: English

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