Abstract：
:Ni/Fe oxyhydroxides are the best performing Earth-abundant electrocatalysts for water oxidation. However, the origin of their remarkable performance is not well understood. Herein, we employ spectroelectrochemical techniques to analyse the kinetics of water oxidation on a series of Ni/Fe oxyhydroxide films: FeOOH, FeOOHNiOOH, and Ni(Fe)OOH (5% Fe). The concentrations and reaction rates of the oxidised states accumulated during catalysis are determined. Ni(Fe)OOH is found to exhibit the fastest reaction kinetics but accumulates fewer states, resulting in a similar performance to FeOOHNiOOH. The later catalytic onset in FeOOH is attributed to an anodic shift in the accumulation of oxidised states. Rate law analyses reveal that the rate limiting step for each catalyst involves the accumulation of four oxidised states, Ni-centred for Ni(Fe)OOH but Fe-centred for FeOOH and FeOOHNiOOH. We conclude by highlighting the importance of equilibria between these accumulated species and reactive intermediates in determining the activity of these materials.
journal_name
Nat Communjournal_title
Nature communicationsauthors
Francàs L,Corby S,Selim S,Lee D,Mesa CA,Godin R,Pastor E,Stephens IEL,Choi KS,Durrant JRdoi
10.1038/s41467-019-13061-0subject
Has Abstractpub_date
2019-11-15 00:00:00pages
5208issue
1issn
2041-1723pii
10.1038/s41467-019-13061-0journal_volume
10pub_type
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