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",
publisher = "society of photo optical instrumentation engineers (spie)",
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",

}

RIS

TY - JOUR

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

A1 - Hou,Yidong

A1 - Abrams,Billie L.

A1 - Vesborg,Peter Christian Kjærgaard

A1 - Björketun,Mårten

A1 - Herbst,Konrad

A1 - Bech,Lone

A1 - Seger,Brian

A1 - Pedersen,Thomas

A1 - Hansen,Ole

A1 - Rossmeisl,Jan

A1 - Dahl,Søren

A1 - Nørskov,Jens Kehlet

A1 - Chorkendorff,Ib

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

PB - society of photo optical instrumentation engineers (spie)

PY - 2012

Y1 - 2012

N2 - <p>The influence of the cluster-core unit in cluster-decorated <em>p</em>-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 <em>A</em><sub>3</sub>S<sub>4</sub> or A<sub>3</sub>BS<sub>4</sub> (<em>A</em> = W, Mo; <em>B</em> = Co, Cu). We find that the Mo-based (<em>A</em> = Mo) cluster-decorated Si photoelectrodes show higher PEC performance than otherwise equivalent W-based (<em>A</em> = W) cluster-decorated ones. This is consistent with higher electrocatalytic activity of the Mo-based clusters supported on <em>n</em>-Si when measured in the dark. The result of stability tests is that photoelectrodes decorated with clusters without Co (<em>B</em> not equal Co) can exhibit promising stability, whereas clusters of the structure A<sub>3</sub>CoS<sub>4</sub> (<em>A</em> = 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 A<sub>3</sub>CoS<sub>4</sub> 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.</p>

AB - <p>The influence of the cluster-core unit in cluster-decorated <em>p</em>-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 <em>A</em><sub>3</sub>S<sub>4</sub> or A<sub>3</sub>BS<sub>4</sub> (<em>A</em> = W, Mo; <em>B</em> = Co, Cu). We find that the Mo-based (<em>A</em> = Mo) cluster-decorated Si photoelectrodes show higher PEC performance than otherwise equivalent W-based (<em>A</em> = W) cluster-decorated ones. This is consistent with higher electrocatalytic activity of the Mo-based clusters supported on <em>n</em>-Si when measured in the dark. The result of stability tests is that photoelectrodes decorated with clusters without Co (<em>B</em> not equal Co) can exhibit promising stability, whereas clusters of the structure A<sub>3</sub>CoS<sub>4</sub> (<em>A</em> = 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 A<sub>3</sub>CoS<sub>4</sub> 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.</p>

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

JO - Journal of Photonics for Energy

JF - Journal of Photonics for Energy

SN - 1947-7988

VL - 2

ER -