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

Publication: Research - peer-reviewJournal article – Annual report year: 2012

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@article{353a8ee22a1e42ff8224f2dce4a07525,
title = "Photoelectrocatalysis and electrocatalysis on silicon electrodes decorated with cubane-like clusters",
keywords = "Cubane-like cluster, Silicon, Photocathode, Hydrogen evolution, Density functional theory, Photoelectrochemical",
author = "Yidong Hou and Abrams, {Billie L.} and Vesborg, {Peter Christian Kjærgaard} and Mårten Björketun and Konrad Herbst and Lone Bech and Brian Seger and Thomas Pedersen and Ole Hansen and Jan Rossmeisl and Søren Dahl and Nørskov, {Jens Kehlet} and Ib Chorkendorff",
note = "Copyright 2012 Society of Photo Optical Instrumentation Engineers",
year = "2012",
doi = "10.1117/1.JPE.2.026001",
volume = "2",
journal = "Journal of Photonics for Energy",
issn = "1947-7988",
publisher = "society of photo optical instrumentation engineers (spie)",

}

RIS

TY - JOUR

T1 - Photoelectrocatalysis and electrocatalysis on silicon electrodes decorated with cubane-like clusters

AU - Hou,Yidong

AU - Abrams,Billie L.

AU - Vesborg,Peter Christian Kjærgaard

AU - Björketun,Mårten

AU - Herbst,Konrad

AU - Bech,Lone

AU - Seger,Brian

AU - Pedersen,Thomas

AU - Hansen,Ole

AU - Rossmeisl,Jan

AU - Dahl,Søren

AU - Nørskov,Jens Kehlet

AU - Chorkendorff,Ib

N1 - Copyright 2012 Society of Photo Optical Instrumentation Engineers

PY - 2012

Y1 - 2012

N2 - The influence of the cluster-core unit in cluster-decorated p-Si on photoelectrochemical (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 (B not equal 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.

AB - The influence of the cluster-core unit in cluster-decorated p-Si on photoelectrochemical (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 (B not equal 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.

KW - Cubane-like cluster

KW - Silicon

KW - Photocathode

KW - Hydrogen evolution

KW - Density functional theory

KW - Photoelectrochemical

U2 - 10.1117/1.JPE.2.026001

DO - 10.1117/1.JPE.2.026001

M3 - Journal article

VL - 2

JO - Journal of Photonics for Energy

T2 - Journal of Photonics for Energy

JF - Journal of Photonics for Energy

SN - 1947-7988

ER -