Solar Fuel and Solar Hydrogen

Photoelectrocatalysis and electrocatalysis on silicon electrodes decorated with cubane-like clusters

[+] Author Affiliations
Yidong Hou

Technical University of Denmark, CINF, Department of Physics, DK-2800 Kongens Lyngby, Denmark

Billie L. Abrams, Konrad Herbst

Haldor Topsøe A/S, Nymøllevej 55, DK-2800 Kongens Lyngby, Denmark

Peter C.K. Vesborg, Lone Bech

Technical University of Denmark, CINF, Department of Physics, DK-2800 Kongens Lyngby, Denmark

Mårten E. Björketun

Technical University of Denmark, CAMD, Department of Physics, DK-2800 Kongens Lyngby, Denmark

Brian Seger

Technical University of Denmark, CINF, Department of Physics, DK-2800 Kongens Lyngby, Denmark

Thomas Pedersen

Technical University of Denmark, Department of Micro- and Nanotechnology, DK-2800 Kongens Lyngby, Denmark

Ole Hansen

Technical University of Denmark, Department of Micro- and Nanotechnology, DK-2800 Kongens Lyngby, Denmark

Jan Rossmeisl

Technical University of Denmark, CAMD, Department of Physics, DK-2800 Kongens Lyngby, Denmark

Søren Dahl

Technical University of Denmark, CINF, Department of Physics, DK-2800 Kongens Lyngby, Denmark

Jens K. Nørskov

Technical University of Denmark, CAMD, Department of Physics, DK-2800 Kongens Lyngby, Denmark

Stanford University, Department of Chemical Engineering, Stanford, California 94305

Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025

Ib Chorkendorff

Technical University of Denmark, CINF, Department of Physics, DK-2800 Kongens Lyngby, Denmark

J. Photon. Energy. 2(1), 026001 (Mar 19, 2012). doi:10.1117/1.JPE.2.026001
History: Received October 11, 2011; Revised December 23, 2011; Accepted January 31, 2012
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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 A3BS4 (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 (BCo) 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.

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© 2012 Society of Photo-Optical Instrumentation Engineers

Citation

Yidong Hou ; Billie L. Abrams ; Peter C.K. Vesborg ; Mårten E. Björketun ; Konrad Herbst, et al.
"Photoelectrocatalysis and electrocatalysis on silicon electrodes decorated with cubane-like clusters", J. Photon. Energy. 2(1), 026001 (Mar 19, 2012). ; http://dx.doi.org/10.1117/1.JPE.2.026001


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