A scanning probe investigation of the role of surface motifs in the behavior of p-WSe2 photocathodes

Velazquez, Jesus M.; John, Jimmy; Esposito, Daniel V.; Pieterick, Adam; Pala, Ragip; Sun, Guofeng; Zhou, Xinghao; Huang, Zhuangqun; Ardo, Shane; Soriaga, Manuel P.; Brunschwig, Bruce S.; Lewis, Nathan S.

doi:10.1039/c5ee02530c

Title: A scanning probe investigation of the role of surface motifs in the behavior of p-WSe₂ photocathodes

Journal Article · Thu Oct 08 00:00:00 EDT 2015 · Energy & Environmental Science

DOI:https://doi.org/10.1039/c5ee02530c· OSTI ID:1436126

Velazquez, Jesus M. ^[1];

^[2]; Esposito, Daniel V. ^[3]; Pieterick, Adam ^[4]; Pala, Ragip ^[4]; Sun, Guofeng ^[5]; Zhou, Xinghao ^[4]; Huang, Zhuangqun ^[6]; Ardo, Shane ^[7]; Soriaga, Manuel P. ^[5]; Brunschwig, Bruce S. ^[8]; Lewis, Nathan S. ^[9]

California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Chemistry and Chemical Engineering; California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP)
California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Chemistry and Chemical Engineering
Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering; National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Neutron Research. Materials Measurement Lab.
California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP); California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Engineering and Applied Science
California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP)
Bruker Nano Surfaces, Goleta, CA (United States)
Univ. of California, Irvine, CA (United States). Dept. of Chemistry and Department of Chemical Engineering and Materials Science
California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP); California Inst. of Technology (CalTech), Pasadena, CA (United States). Molecular Materials Research Center, Beckman Inst.
California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Chemistry and Chemical Engineering; California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP); California Inst. of Technology (CalTech), Pasadena, CA (United States). Molecular Materials Research Center, Beckman Inst.; California Inst. of Technology (CalTech), Pasadena, CA (United States). Kavli Nanoscience Inst.

The spatial variation in the photoelectrochemical performance for the reduction of an aqueous one-electron redox couple, Ru(NH₃)₆^3+/2+, and for the evolution of H₂(g) from 0.5 M H₂SO₄(aq) at the surface of bare or Pt-decorated p-type WSe₂ photocathodes has been investigated in situ using scanning photocurrent microscopy (SPCM). The measurements revealed significant differences in the charge-collection performance (quantified by the values of external quantum yields, Φ_ext) on various macroscopic terraces. Local spectral response measurements indicated a variation in the local electronic structure among the terraces, which was consistent with a non-uniform spatial distribution of sub-band-gap states within the crystals. The photoconversion efficiencies of Pt-decorated p-WSe2 photocathodes were greater for the evolution of H₂(g) from 0.5 M H₂SO₄ than for the reduction of Ru(NH₃)₆^3+/2+, and terraces that exhibited relatively low values of Φext for the reduction of Ru(NH₃)₆^3+/2+ could in some cases yield values of Φ_ext for the evolution of H₂(g) comparable to the values of Φ_ext yielded by the highest-performing terraces. In conclusion, although the spatial resolution of the techniques used in this work frequently did not result in observation of the effect of edge sites on photocurrent efficiency, some edge effects were observed in the measurements; however the observed edge effects differed among edges, and did not appear to determine the performance of the electrodes.

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Research Organization:: California Institute of Technology (CalTech), Pasadena, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office (HFTO)

Grant/Contract Number:: SC0004993; FG02-03ER15483

OSTI ID:: 1436126

Journal Information:: Energy & Environmental Science, Vol. 9, Issue 1; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 32 works

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Layer dependence of the photoelectrochemical performance of a WSe ₂ photocathode characterized using in situ microscale measurements Zhang, Yu; Xiao, Jingwei; Xie, Xi RSC Advances, Vol. 9, Issue 53 https://doi.org/10.1039/c9ra06297a	journal	January 2019
Depletion layer controls photocatalytic hydrogen evolution with p-type gallium phosphide particles Zhao, Zeqiong; Willard, Emma J.; Dominguez, Julius R. Journal of Materials Chemistry A, Vol. 7, Issue 30 https://doi.org/10.1039/c9ta05879f	journal	January 2019
Two-Dimensional Material Molybdenum Disulfides as Electrocatalysts for Hydrogen Evolution Yang, Lei; Liu, Ping; Li, Jing Catalysts, Vol. 7, Issue 10 https://doi.org/10.3390/catal7100285	journal	September 2017
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Title: A scanning probe investigation of the role of surface motifs in the behavior of p-WSe₂ photocathodes