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@article{Lin:2022:10.1039/d1ee03522c,
author = {Lin, R and Kang, L and Zhao, T and Feng, J and Celorrio, V and Zhang, G and Cibin, G and Kucernak, A and Brett, DJL and Corà, F and Parkin, IP and He, G},
doi = {10.1039/d1ee03522c},
journal = {Energy and Environmental Science},
pages = {2386--2396},
title = {Identification and manipulation of dynamic active site deficiency-induced competing reactions in electrocatalytic oxidation processes},
url = {http://dx.doi.org/10.1039/d1ee03522c},
volume = {15},
year = {2022}
}

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TY  - JOUR
AB  - Electrocatalytic organic compound oxidation reactions (OCORs) have been intensively studied for energy and environmentally benign applications. However, relatively little effort has been devoted to developing a fundamental understanding of OCORs, including the detailed competition with side reactions and activity limitations, thus inhibiting the rational design of high-performance electrocatalysts. Herein, by taking the NiWO4-catalysed urea oxidation reaction (UOR) in aqueous media as an example, the competition between the OCOR and the oxygen evolution reaction (OER) within a wide potential range is examined. It is shown that the root of the competition can be ascribed to insufficient surface concentration of dynamic Ni3+, an active site shared by both the UOR and OER. A similar phenomenon is observed in other OCOR electrocatalysts and systems. To address the issue, a “controllable reconstruction of pseudo-crystalline bimetal oxides” design strategy is proposed to maximise the dynamic Ni3+ population and manipulate the competition between the UOR and the OER. The optimised electrocatalyst delivers best-in-class performance and an ∼10-fold increase in current density at 1.6 V versus the reversible hydrogen electrode for alkaline urea electrolysis compared to those of the pristine materials.
AU  - Lin,R
AU  - Kang,L
AU  - Zhao,T
AU  - Feng,J
AU  - Celorrio,V
AU  - Zhang,G
AU  - Cibin,G
AU  - Kucernak,A
AU  - Brett,DJL
AU  - Corà,F
AU  - Parkin,IP
AU  - He,G
DO  - 10.1039/d1ee03522c
EP  - 2396
PY  - 2022///
SN  - 1754-5692
SP  - 2386
TI  - Identification and manipulation of dynamic active site deficiency-induced competing reactions in electrocatalytic oxidation processes
T2  - Energy and Environmental Science
UR  - http://dx.doi.org/10.1039/d1ee03522c
UR  - https://pubs.rsc.org/en/content/articlelanding/2022/EE/D1EE03522C
UR  - http://hdl.handle.net/10044/1/96648
VL  - 15
ER  -

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