Journal
ENERGY & FUELS
Volume 35, Issue 23, Pages 19164-19169Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.energyfuels.1c02674
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Funding
- Arnold and Mabel Beckman Foundation
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This study discusses the active sites in nickel-iron water oxidation electrocatalysts, suggesting that iron is a likely candidate for highly active materials whereas nickel is likely not the active site for water oxidation electrocatalysis. The conclusion is supported by three-fold arguments based on electrochemical measurements.
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.
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