Enhancing Hydrogen Evolution Reaction via Synergistic Interaction between the [Mo3S13]2- Cluster Co-Catalyst and WSe2 Photocathode

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)2Mo3S13 solution both on FTO glass substrates as hydrogen evolving electrodes and on highly 00.1-textured WSe2 for photoelectrochemical water splitting. As an electrocatalyst, [Mo3S13]2- clusters demonstrate a low overpotential of 220 mV at 10 mA cm-2 in 0.5 M H2SO4 electrolyte (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-2 at 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 WSe2 support, 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.

Medienart:

E-Artikel

Erscheinungsjahr:

2022

Erschienen:

2022

Enthalten in:

Zur Gesamtaufnahme - volume:14

Enthalten in:

ACS applied materials & interfaces - 14(2022), 47 vom: 30. Nov., Seite 52815-52824

Sprache:

Englisch

Beteiligte Personen:

Xi, Fanxing [VerfasserIn]
Bozheyev, Farabi [VerfasserIn]
Han, Xiaoyu [VerfasserIn]
Rusu, Marin [VerfasserIn]
Rappich, Jörg [VerfasserIn]
Abdi, Fatwa F [VerfasserIn]
Bogdanoff, Peter [VerfasserIn]
Kaltsoyannis, Nikolas [VerfasserIn]
Fiechter, Sebastian [VerfasserIn]

Links:

Volltext

Themen:

Heterojunction
Hydrogen evolving catalyst
Journal Article
Molybdenum sulfide
Photoelectrochemistry
Solar water splitting

Anmerkungen:

Date Revised 05.12.2022

published: Print-Electronic

Citation Status PubMed-not-MEDLINE

doi:

10.1021/acsami.2c14312

funding:

Förderinstitution / Projekttitel:

PPN (Katalog-ID):

NLM348928939