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Journal of Photonics for Energy

Photoelectrocatalysis and electrocatalysis on silicon electrodes decorated with cubane-like clusters
Author(s): Yidong Hou; Peter C. Vesborg; Lone Bech; Brian Seger; Søren Dahl; Ib Chorkendorff; Billie L. Abrams; Konrad Herbst; Marten Bjørketun; Jan Rossmeisl; Jens K. Nørskov; Thomas Pedersen; Ole Hansen
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Paper Abstract

The influence of the cluster-core unit in cluster-decorated p-Si on photo-electrochemical (PEC) hydrogen evolution has been investigated using a homologous series of cubane-like heterobimetallic sulfide compounds. These compounds stem from the generic cluster structure A3S4 or A3B?startSend?4 (A = W, Mo; B = Co, Cu). We find that the Mo-based (A = Mo) cluster-decorated Si photoelectrodes show higher PEC performance than otherwise equivalent W-based (A = W) cluster-decorated ones. This is consistent with higher electrocatalytic activity of the Mo-based clusters supported on n-Si when measured in the dark. The result of stability tests is that photoelectrodes decorated with clusters without Co (B ≠ Co) can exhibit promising stability, whereas clusters of the structure A3CoS4  (A = W, Mo) yield photoelectrodes that are highly unstable upon illumination. X-ray photoelectron spectroscopy (XPS) results suggest that both oxidation and material loss play a role in deactivation of the A3CoS4 materials. Additionally, we observe that the photocurrent depends linearly on the light intensity in the limiting current region, and the corresponding incident photon to current efficiency (IPCE) may reach approximately 80%. Density functional theory (DFT) calculations of the clusters adsorbed on the hydrogen-terminated Si surface are used to estimate and compare cluster adsorption energies on the surface as well as the H-binding energies, which is a descriptor for electrocatalytic activity.

Paper Details

Date Published: 19 March 2012
PDF: 17 pages
J. Photon. Energy 2(1) 026001 doi: 10.1117/1.JPE.2.026001
Published in: Journal of Photonics for Energy Volume 2, Issue 1
Show Author Affiliations
Yidong Hou, Technical Univ. of Denmark (Denmark)
Peter C. Vesborg, Technical Univ. of Denmark (Denmark)
Lone Bech, Technical Univ. of Denmark (Denmark)
Brian Seger, Technical Univ. of Denmark (Denmark)
Søren Dahl, Technical Univ. of Denmark (Denmark)
Ib Chorkendorff, Technical Univ. of Denmark (Denmark)
Billie L. Abrams, Topsoe Fuel Cell (Denmark)
Konrad Herbst, Topsoe Fuel Cell (Denmark)
Marten Bjørketun, Technical Univ. of Denmark (Denmark)
Jan Rossmeisl, Technical Univ. of Denmark (Denmark)
Jens K. Nørskov, Technical Univ. of Denmark (Denmark)
Thomas Pedersen, Technical Univ. of Denmark (Denmark)
Ole Hansen, Technical Univ. of Denmark (Denmark)

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