Abstract
The poor activity and stability of electrode materials for the oxygen evolution reaction are the main bottlenecks in the water-splitting reaction for H2 production. Here, by studying the activity–stability trends for the oxygen evolution reaction on conductive M1OxHy, Fe–M1OxHy and Fe–M1M2OxHy hydr(oxy)oxide clusters (M1 = Ni, Co, Fe; M2 = Mn, Co, Cu), we show that balancing the rates of Fe dissolution and redeposition over a MOxHy host establishes dynamically stable Fe active sites. Together with tuning the Fe content of the electrolyte, the strong interaction of Fe with the MOxHy host is the key to controlling the average number of Fe active sites present at the solid/liquid interface. We suggest that the Fe–M adsorption energy can therefore serve as a reaction descriptor that unifies oxygen evolution reaction catalysis on 3d transition-metal hydr(oxy)oxides in alkaline media. Thus, the introduction of dynamically stable active sites extends the design rules for creating active and stable interfaces.
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Data availability
All data are available in the main text, Supplementary Information and Source Data files. Data generated from DFT calculations can be found in Supplementary Data 1.
Change history
03 June 2020
A Correction to this paper has been published: https://doi.org/10.1038/s41560-020-0638-1
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Acknowledgements
The research was carried out at Argonne National Laboratory and supported by the Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division. Use of the Center for Nanoscale Materials and the Advanced Photon Source, Office of Science user facilities, was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357. T.K. thanks the Japan Society for the Promotion of Science for Postdoctoral Fellowship. H.H. acknowledges the funding support from the Visiting Faculty Program of the Department of Energy.
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D.Y.C., P.P.L. and N.M.M. designed the experiments. D.Y.C., P.P.L. and P.F.B.D.M. conducted the electrochemical measurements and analysis. H.H. and P.Z. performed DFT calculations and analysis. D.Y.C., T.K., H.Y., S.S. and S.L. conducted in situ XANES measurements and analysis. D.T. and Y.Z. carried out STM and AFM analyses. D.S. and V.R.S. discussed and commented on the results. D.Y.C., P.P.L., P.Z. and N.M.M. wrote the manuscript. All authors approved the final version of the manuscript.
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Chung, D.Y., Lopes, P.P., Farinazzo Bergamo Dias Martins, P. et al. Dynamic stability of active sites in hydr(oxy)oxides for the oxygen evolution reaction. Nat Energy 5, 222–230 (2020). https://doi.org/10.1038/s41560-020-0576-y
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DOI: https://doi.org/10.1038/s41560-020-0576-y
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