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Mechanism of Nickel–Iron Water Oxidation Electrocatalysts

Zhang, Jibo and Winkler, Jay R. and Gray, Harry B. and Hunter, Bryan M. (2021) Mechanism of Nickel–Iron Water Oxidation Electrocatalysts. Energy and Fuels . ISSN 0887-0624. doi:10.1021/acs.energyfuels.1c02674. (In Press) https://resolver.caltech.edu/CaltechAUTHORS:20211008-224627576

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Abstract

Hotly debated these days is whether nickel or iron is the active site in nickel–iron water oxidation electrocatalysts. We have previously argued that iron is a likely candidate for highly active materials because it can reach high-oxidation (high-ox) states at potentials relevant to water splitting. Here, we further assert that nickel is likely not an active site for water oxidation electrocatalysis in these materials. Our 3-fold argument is supported by electrochemical measurements on rigorously planar electrodes produced by pulsed laser ablation in liquids: (1) nickel cannot achieve high-ox states in aqueous environments at relevant potentials; (2) large steady-state concentrations of metal sites preclude them from being active, thereby indicating that even more oxidizing moieties are critically important; and (3) unlike nickel sites, high-ox iron sites documented experimentally are neither rare nor unreasonably reactive.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acs.energyfuels.1c02674DOIArticle
ORCID:
AuthorORCID
Winkler, Jay R.0000-0002-4453-9716
Gray, Harry B.0000-0002-7937-7876
Hunter, Bryan M.0000-0001-8559-9304
Additional Information:© 2021 The Authors. Published by American Chemical Society. Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0) Received 5 August 2021. Published online 23 September 2021. This article is part of the 2021 Pioneers in Energy Research: Vivian Yam special issue. Bryan M. Hunter is a Fellow of the Rowland Institute at Harvard University. The authors thank the Arnold and Mabel Beckman Foundation for support of their work. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
Rowland InstituteUNSPECIFIED
Arnold and Mabel Beckman FoundationUNSPECIFIED
Subject Keywords:Iron, Radiology, Electrodes, Water oxidation, Nickel
DOI:10.1021/acs.energyfuels.1c02674
Record Number:CaltechAUTHORS:20211008-224627576
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20211008-224627576
Official Citation:Mechanism of Nickel–Iron Water Oxidation Electrocatalysts Jibo Zhang, Jay R. Winkler, Harry B. Gray, and Bryan M. Hunter Energy & Fuels Article ASAP DOI: 10.1021/acs.energyfuels.1c02674
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:111330
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:11 Oct 2021 23:02
Last Modified:11 Oct 2021 23:02

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