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research article

Spectroelectrochemical analysis of the mechanism of (photo)electrochemical hydrogen evolution at a catalytic interface

Pastor, Ernest
•
Le Formal, Florian  
•
Mayer, Matthew T.  
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2017
Nature Communications

Multi-electron heterogeneous catalysis is a pivotal element in the ( photo) electrochemical generation of solar fuels. However, mechanistic studies of these systems are difficult to elucidate by means of electrochemical methods alone. Here we report a spectro-electrochemical analysis of hydrogen evolution on ruthenium oxide employed as an electrocatalyst and as part of a cuprous oxide-based photocathode. We use optical absorbance spectroscopy to quantify the densities of reduced ruthenium oxide species, and correlate these with current densities resulting from proton reduction. This enables us to compare directly the catalytic function of dark and light electrodes. We find that hydrogen evolution is second order in the density of active, doubly reduced species independent of whether these are generated by applied potential or light irradiation. Our observation of a second order rate law allows us to distinguish between the most common reaction paths and propose a mechanism involving the homolytic reductive elimination of hydrogen.

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Type
research article
DOI
10.1038/ncomms14280
Web of Science ID

WOS:000394643200001

Author(s)
Pastor, Ernest
Le Formal, Florian  
Mayer, Matthew T.  
Tilley, S. David  
Francas, Laia
Mesa, Camilo A.
Gratzel, Michael  
Durrant, James R.
Date Issued

2017

Publisher

Springer Nature

Published in
Nature Communications
Volume

8

Article Number

14280

Note

This article is licensed under a Creative Commons Attribution 4.0 International License

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LPI  
Available on Infoscience
March 27, 2017
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/135855
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