Enhancing Hydrogen Evolution Reaction via Synergistic Interaction between the [Mo3S13]2-Cluster Co-Catalyst and WSe2Photocathode
Xi F. Bozheyev F. Han X. Rusu M. Rappich J. Abdi F.F. Bogdanoff P. Kaltsoyannis N. Fiechter S.
30 November 2022American Chemical Society
ACS Applied Materials and Interfaces
2022#14Issue 4752815 - 52824 pp.
A thiomolybdate [Mo3S13]2-nanocluster is a promising catalyst for hydrogen evolution reaction (HER) due to the high number of active edge sites. In this work, thiomolybdate cluster films are prepared by spin-coating of a (NH4)2Mo3S13solution both on FTO glass substrates as hydrogen evolving electrodes and on highly 00.1-textured WSe2for photoelectrochemical water splitting. As an electrocatalyst, [Mo3S13]2-clusters demonstrate a low overpotential of 220 mV at 10 mA cm-2in 0.5 M H2SO4electrolyte (pH 0.3) and remain structurally stable during the electrochemical cycling as revealed by in situ Raman spectroscopy. Moreover, as a co-catalyst on WSe2, [Mo3S13]2-clusters enhance the photocurrent substantially by more than two orders of magnitude (from 0.02 to 2.8 mA cm-2at 0 V vs RHE). The synergistic interactions between the photoelectrode and catalyst, i.e., surface passivation and band bending modification by the [Mo3S13]2-cluster film, promoted HER catalytic activity of [Mo3S13]2-clusters influenced by the WSe2support, are revealed by intensity-modulated photocurrent spectroscopy and density functional theory calculations, respectively. The band alignment of the WSe2/[Mo3S13]2-heterojunction, which facilitates the electron injection, is determined by correlating UV-vis with photoelectron yield spectroscopy results.
heterojunction , hydrogen evolving catalyst , molybdenum sulfide , photoelectrochemistry , solar water splitting
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Institute for Solar Fuels, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Hahn-Meitner-Platz 1, Berlin, 14109, Germany
Institute of Photoelectrochemistry, Helmholtz-Zentrum Hereon, Geesthacht, 21502, Germany
National Nanolaboratory, Al-Farabi Kazakh National University, 71 al-Farabi Ave., Almaty, 050000, Kazakhstan
Department of Chemistry, The University of Manchester, Oxford Road, Manchester, M13 9PL, United Kingdom
Department Structure and Dynamics of Energy Materials, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Hahn-Meitner-Platz 1, Berlin, 14109, Germany
Institute Silicon Photovoltaics, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Magnusstrasse 12, Berlin, 12489, Germany
PV ComB, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Schwarzschildstrasse 3, Berlin, 12489, Germany
Institute for Solar Fuels
Institute of Photoelectrochemistry
National Nanolaboratory
Department of Chemistry
Department Structure and Dynamics of Energy Materials
Institute Silicon Photovoltaics
PV ComB
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