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Kinetics of light-driven oxygen evolution at alpha-Fe2O3 electrodes.

Laurence M Peter¹, K G Upul Wijayantha, Asif A Tahir

¹Department of Chemistry, University of Bath, Bath, BA2 7AY, United Kingdom. l.m.peter@bath.ac.uk

Faraday Discussions

|April 5, 2012

Summary

Investigating light-driven oxygen evolution in alpha-Fe2O3, this study reveals surface treatment significantly boosts photocurrent by suppressing electron-hole recombination, not by catalyzing water oxidation.

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Area of Science:

Materials Science
Electrochemistry
Photocatalysis

Background:

Polycrystalline alpha-Fe2O3 is a promising material for light-driven oxygen evolution.
Understanding the kinetics and limiting factors is crucial for improving its efficiency.
Surface states and recombination pathways significantly impact photocatalytic performance.

Purpose of the Study:

To investigate the kinetics of light-driven oxygen evolution at alpha-Fe2O3.
To analyze the impact of surface treatment on photocurrent response.
To elucidate the mechanism behind the observed improvements in photocatalytic activity.

Main Methods:

Preparation of polycrystalline alpha-Fe2O3 layers using aerosol-assisted chemical vapour deposition.
Study of reaction kinetics using intensity modulated photocurrent spectroscopy (IMPS).
Analysis of frequency-dependent IMPS data to understand charge carrier dynamics.

Main Results:

Identified slow kinetics for oxygen evolution, indicating a kinetic bottleneck.
Observed a significant improvement in photocurrent response after surface treatment with cobalt nitrate.
Determined that the improvement is due to suppression of surface recombination, not catalysis of hole transfer.

Conclusions:

Surface recombination is a major limiting factor in light-driven oxygen evolution at alpha-Fe2O3.
Surface treatment strategies that minimize recombination are effective for enhancing photocatalytic activity.
The findings provide critical insights for designing more efficient semiconductor photoanodes for water splitting.