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Gold-supported cerium-doped NiOx catalysts for water oxidation

Nature Energy volume 1, Article number: 16053 (2016) Cite this article

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Abstract

The development of high-performance catalysts for the oxygen-evolution reaction (OER) is paramount for cost-effective conversion of renewable electricity to fuels and chemicals. Here we report the significant enhancement of the OER activity of electrodeposited NiOx films resulting from the combined effects of using cerium as a dopant and gold as a metal support. This NiCeOx–Au catalyst delivers high OER activity in alkaline media, and is among the most active OER electrocatalysts yet reported. On the basis of experimental observations and theoretical modelling, we ascribe the activity to a combination of electronic, geometric and support effects, where highly active under-coordinated sites at the oxide support interface are modified by the local chemical binding environment and by doping the host Ni oxide with Ce. The NiCeOx–Au catalyst is further demonstrated in a device context by pairing it with a nickel–molybdenum hydrogen evolution catalyst in a water electrolyser, which delivers 50 mA consistently at 1.5 V over 24 h of continuous operation.

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Figure 1: Physical and chemical characterization of NiCeOx–Au.
Figure 2: Experimental and theoretical OER performance of NiCeOx–Au.
Figure 3: Deconvolution of the various effects modifying the OER performance of NiCeOx–Au.
Figure 4: Evaluation of the performance of NiCeOx–Au in an electrolyser set-up.

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Acknowledgements

This work was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0008685 and the US Department of Energy Office of Basic Energy Science grant to the SUNCAT Center for Interface Science and Catalysis. Partial support to initiate the project was provided as part of the Center on Nanostructuring for Efficient Energy Conversion (CNEEC) at Stanford University, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0001060. The authors would like to thank L. Seitz for helpful discussions and R. Kravec for help with XRD measurements. J.W.D.N. acknowledges funding from the Agency of Science, Technology, and Research (A∗STAR), Singapore. M.G.-M. acknowledges funding from the Agency for Administration of University and Research Grants of Catalonia (AGAUR, 2013 BP-A 00464). C.K. acknowledges funding from the Stanford Graduate Fellowship. A.V. acknowledges funding through the SLAC National Accelerator Laboratory LDRD Program.

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Authors and Affiliations

  1. Department of Chemical Engineering, Stanford University, Stanford, California 94305, USA

    Jia Wei Desmond Ng, Pongkarn Chakthranont, Charlotte Kirk & Thomas F. Jaramillo

  2. SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA

    Max García-Melchor, Michal Bajdich, Aleksandra Vojvodic & Thomas F. Jaramillo

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Contributions

J.W.D.N. and T.F.J. conceived and designed the experiments. J.W.D.N., P.C. and C.K. carried out material synthesis. J.W.D.N. and P.C. performed physical and chemical characterization. J.W.D.N., P.C. and C.K. conducted the electrochemical measurements. M.G.-M., M.B. and A.V. formulated, defined and designed the computational part of the paper. M.G.-M. and M.B. performed all the DFT calculations under supervision from A.V. All authors discussed the results and co-wrote the paper.

Corresponding authors

Correspondence to Aleksandra Vojvodic or Thomas F. Jaramillo.

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Supplementary Figures 1–13, Supplementary Table 1, Supplementary Discussion and Supplementary References. (PDF 2277 kb)

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Ng, J., García-Melchor, M., Bajdich, M. et al. Gold-supported cerium-doped NiOx catalysts for water oxidation. Nat Energy 1, 16053 (2016). https://doi.org/10.1038/nenergy.2016.53

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