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Highly active and low-cost catalysts for electrochemical reactions such as the hydrogen evolution reaction (HER) are crucial for the development of efficient energy conversion and storage technologies. Theoretical simulations have been instrumental in revealing the correlations between the electronic structure of materials and their catalytic activity, and guide the prediction and development of improved catalysts. However, difficulties in accurately engineering the desired atomic sites lead to challenges in making direct comparisons between experimental and theoretical results. In MoS2, the Mo-edge has been demonstrated to be active for HER whereas the S-edge is inert. Using a computational descriptor-based approach, we predict that by incorporating transition metal atoms (Fe, Co, Ni, or Cu) the S-edge site should also become HER active. Vertically standing, edge-terminated MoS2 nanofilms provide a well-defined model system for verifying these predictions. The transition metal doped MoS2 nanofilms show an increase in exchange current densities by at least two-fold, in agreement with the theoretical calculations. This work opens up further opportunities for improving electrochemical catalysts by incorporating promoters into particular atomic sites, and for using well-defined systems in order to understand the origin of the promotion effects.

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Publication history
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Acknowledgements

Publication history

Received: 06 October 2014
Revised: 30 November 2014
Accepted: 02 December 2014
Published: 27 January 2015
Issue date: February 2015

Copyright

© Tsinghua University Press and Springer‐Verlag Berlin Heidelberg 2014

Acknowledgements

Acknowledgements

H.W., D.K. and Y.C. acknowledge support by the Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under contract DE-AC02-76-SFO0515. C.T., K.C., F.A-P., and J.K.N. acknowledge support from the Center on Nanostructuring for Efficient Energy Conversion (CNEEC) at Stanford University, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Basic Energy Sciences under award number DE-SC0001060. F.A.-P. and J.K.N. acknowledge financial support from the U.S. Department of Energy, Office of Basic Energy Sciences to the SUNCAT Center for Interface Science and Catalysis. C.T. acknowledges financial support from the NSF GRFP Grant DGE- 114747.

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