Abstract
Highly (00.1)-textured polycrystalline WSe 2 films are developed as hydrogen evolving photoelectrodes and improved through deposition of a thin ammonium thiomolybdate (NH 4 ) 2 Mo 3 S 13 catalyst film. This semiconducting thiomolybdate forms a heterojunction with the p-type WSe 2 film passivating recombination centers of excited electron-hole pairs at the edges of the (00.1) textured WSe 2 nanoflakes. In addition, thiomolybdate acts as a photoelectrocatalyst at the electrode-aqueous electrolyte interface during light-driven hydrogen evolution. Whereas the photoelectrochemical activity of pure WSe 2 is dominated by charge carrier recombination processes at edge states of the hexagonal nanoflakes, we obtain homogeneous charge transfer across the van der Waals planes concomitant with the passivation of these edge states. A photocurrent density of up to 5.6 mA cm -2 at 0 V vs. RHE is obtained with the proposed homogeneously distributed (NH 4 ) 2 Mo 3 S 13 /WSe 2 heterojunction system under AM 1.5 illumination in the 0.5 M H 2 SO 4 electrolyte. We conclude that homogeneously distributed semiconducting catalysts on the van der Waals planes of WSe 2 nano-crystallites are a feasible strategy towards solar hydrogen evolution with large-area photoelectrocathodes.
| Original language | English |
|---|---|
| Pages (from-to) | 10769-10780 |
| Number of pages | 12 |
| Journal | Journal of Materials Chemistry A |
| Volume | 7 |
| Issue number | 17 |
| DOIs | |
| Publication status | Published - Jan 1 2019 |
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ASJC Scopus subject areas
- Chemistry(all)
- Renewable Energy, Sustainability and the Environment
- Materials Science(all)
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Efficient charge transfer at a homogeneously distributed (NH 4 ) 2 Mo 3 S 13 /WSe 2 heterojunction for solar hydrogen evolution . / Bozheyev, Farabi; Xi, Fanxing; Plate, Paul; Dittrich, Thomas; Fiechter, Sebastian; Ellmer, Klaus.
In: Journal of Materials Chemistry A, Vol. 7, No. 17, 01.01.2019, p. 10769-10780.Research output: Contribution to journal › Article
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TY - JOUR
T1 - Efficient charge transfer at a homogeneously distributed (NH 4 ) 2 Mo 3 S 13 /WSe 2 heterojunction for solar hydrogen evolution
AU - Bozheyev, Farabi
AU - Xi, Fanxing
AU - Plate, Paul
AU - Dittrich, Thomas
AU - Fiechter, Sebastian
AU - Ellmer, Klaus
PY - 2019/1/1
Y1 - 2019/1/1
N2 - Highly (00.1)-textured polycrystalline WSe 2 films are developed as hydrogen evolving photoelectrodes and improved through deposition of a thin ammonium thiomolybdate (NH 4 ) 2 Mo 3 S 13 catalyst film. This semiconducting thiomolybdate forms a heterojunction with the p-type WSe 2 film passivating recombination centers of excited electron-hole pairs at the edges of the (00.1) textured WSe 2 nanoflakes. In addition, thiomolybdate acts as a photoelectrocatalyst at the electrode-aqueous electrolyte interface during light-driven hydrogen evolution. Whereas the photoelectrochemical activity of pure WSe 2 is dominated by charge carrier recombination processes at edge states of the hexagonal nanoflakes, we obtain homogeneous charge transfer across the van der Waals planes concomitant with the passivation of these edge states. A photocurrent density of up to 5.6 mA cm -2 at 0 V vs. RHE is obtained with the proposed homogeneously distributed (NH 4 ) 2 Mo 3 S 13 /WSe 2 heterojunction system under AM 1.5 illumination in the 0.5 M H 2 SO 4 electrolyte. We conclude that homogeneously distributed semiconducting catalysts on the van der Waals planes of WSe 2 nano-crystallites are a feasible strategy towards solar hydrogen evolution with large-area photoelectrocathodes.
AB - Highly (00.1)-textured polycrystalline WSe 2 films are developed as hydrogen evolving photoelectrodes and improved through deposition of a thin ammonium thiomolybdate (NH 4 ) 2 Mo 3 S 13 catalyst film. This semiconducting thiomolybdate forms a heterojunction with the p-type WSe 2 film passivating recombination centers of excited electron-hole pairs at the edges of the (00.1) textured WSe 2 nanoflakes. In addition, thiomolybdate acts as a photoelectrocatalyst at the electrode-aqueous electrolyte interface during light-driven hydrogen evolution. Whereas the photoelectrochemical activity of pure WSe 2 is dominated by charge carrier recombination processes at edge states of the hexagonal nanoflakes, we obtain homogeneous charge transfer across the van der Waals planes concomitant with the passivation of these edge states. A photocurrent density of up to 5.6 mA cm -2 at 0 V vs. RHE is obtained with the proposed homogeneously distributed (NH 4 ) 2 Mo 3 S 13 /WSe 2 heterojunction system under AM 1.5 illumination in the 0.5 M H 2 SO 4 electrolyte. We conclude that homogeneously distributed semiconducting catalysts on the van der Waals planes of WSe 2 nano-crystallites are a feasible strategy towards solar hydrogen evolution with large-area photoelectrocathodes.
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U2 - 10.1039/c9ta01220f
DO - 10.1039/c9ta01220f
M3 - Article
VL - 7
SP - 10769
EP - 10780
JO - Journal of Materials Chemistry A
JF - Journal of Materials Chemistry A
SN - 2050-7488
IS - 17
ER -