Ultra-thin Al<inf>2</inf>O<inf>3</inf>coatings on BiVO<inf>4</inf>photoanodes: Impact on performance and charge carrier dynamics
File(s)Manuscript_ammended_2.docx (2.99 MB)
Accepted version
Author(s)
Type
Journal Article
Abstract
Bismuth vanadate (BiVO 4 ) has emerged as one of the most promising photoanode materials for oxidising water due to its visible light activity and low cost. Recent studies have shown that the performance of BiVO 4 photoanodes can be remarkably improved when coated with ultra-thin passivation layers. In this article we investigate the use of ultra-thin Al 2 O 3 layers grown using atomic layer deposition (ALD). At an optimum thickness (~0.33nm, 3 ALD cycles), the Al 2 O 3 layer favourably shifted the onset potential by ~200mV and increased photocatalytic currents for the water oxidation reaction. When held at 1.23V RHE , we observe a remarkable increase in the theoretical solar photocurrent; from ~0.47mAcm -2 in uncoated BiVO 4 to ~3.0mAcm -2 in Al 2 O 3 -coated BiVO 4 . Using transient photocurrent (TPC) and transient absorption spectroscopy (TAS) the charge carrier dynamics in Al 2 O 3 -coated BiVO 4 photoanodes were examined for the first time. TPC showed that photogenerated electrons in the BiVO 4 layer were extracted within ~1ms. TAS showed that the remaining holes oxidised water from ~100ms to 1s. Ultra-thin Al 2 O 3 coatings did not improve the reaction kinetics towards water oxidation, but rather, suppressed bi-molecular recombination on the μs-ms timescale in BiVO 4 , and increased the yield of long-lived holes on the ms-s timescale required to oxidise water. This is attributed to an inhibition of surface recombination on BiVO 4 by Al 2 O 3 , which inhibited the early timescale recombination of charge carriers formed within the space charge layer.
Date Issued
2019-02-01
Date Acceptance
2017-11-08
Citation
Catalysis Today, 2019, 321-322, pp.59-66
ISSN
0920-5861
Publisher
Elsevier
Start Page
59
End Page
66
Journal / Book Title
Catalysis Today
Volume
321-322
Copyright Statement
© 2017, Elsevier. Licensed under the Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International http://creativecommons.org/licenses/by-nc-nd/4.0/
Sponsor
Commission of the European Communities
Grant Number
291482
Subjects
Science & Technology
Physical Sciences
Technology
Chemistry, Applied
Chemistry, Physical
Engineering, Chemical
Chemistry
Engineering
BiVO4 photoanodes
Water oxidation
Water splitting
Ultra-thin Al2O3 coating
Charge carrier dynamics
Transient absorption spectroscopy
BISMUTH VANADATE PHOTOANODES
METAL-OXIDE PHOTOELECTRODES
WATER OXIDATION
PHOTOGENERATED HOLES
QUANTUM EFFICIENCIES
HEMATITE PHOTOANODES
SURFACE PASSIVATION
VISIBLE-LIGHT
FILMS
TIO2
Physical Chemistry
03 Chemical Sciences
09 Engineering
Publication Status
Published
Date Publish Online
2017-11-10