Unveiling charge dynamics of visible light absorbing oxysulfide for efficient overall water splitting

Vikas Nandal (), Ryota Shoji, Hiroyuki Matsuzaki (), Akihiro Furube, Lihua Lin, Takashi Hisatomi, Masanori Kaneko, Koichi Yamashita, Kazunari Domen and Kazuhiko Seki ()
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Vikas Nandal: National Institute of Advanced Industrial Science and Technology (AIST)
Ryota Shoji: National Institute of Advanced Industrial Science and Technology (AIST)
Hiroyuki Matsuzaki: National Institute of Advanced Industrial Science and Technology (AIST)
Akihiro Furube: Tokushima University
Lihua Lin: Shinshu University
Takashi Hisatomi: Shinshu University
Masanori Kaneko: Kyoto University
Koichi Yamashita: Kyoto University
Kazunari Domen: Shinshu University
Kazuhiko Seki: National Institute of Advanced Industrial Science and Technology (AIST)

Nature Communications, 2021, vol. 12, issue 1, 1-8

Abstract: Abstract Oxysulfide semiconductor, Y2Ti2O5S2, has recently discovered its exciting potential for visible-light-induced overall water splitting, and therefore, imperatively requires the probing of unknown fundamental charge loss pathways to engineer the photoactivity enhancement. Herein, transient diffuse reflectance spectroscopy measurements are coupled with theoretical calculations to unveil the nanosecond to microsecond time range dynamics of the photogenerated charge carriers. In early nanosecond range, the pump-fluence-dependent decay dynamics of the absorption signal is originated from the bimolecular recombination of mobile charge carriers, in contrast, the power-law decay kinetics in late microsecond range is dominated by hole detrapping from exponential tail trap states of valence band. A well-calibrated theoretical model estimates various efficiency limiting material parameters like recombination rate constant, n-type doping density and tail-states parameters. Compared to metal oxides, longer effective carrier lifetime ~6 ns is demonstrated. Different design routes are proposed to realize efficiency beyond 10% for commercial solar-to-hydrogen production from oxysulfide photocatalysts.

Date: 2021
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-27199-3

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DOI: 10.1038/s41467-021-27199-3

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