The generation of hydrogen from water and sunlight offers a promising approach for producing scalable and sustainable carbon-free energy. The key of a successful solar-to-fuel technology is the design of efficient, long-lasting and low-cost photoelectrochemical cells, which are responsible for absorbing sunlight and driving water splitting reactions. To this end, a detailed understanding and control of heterogeneous interfaces between photoabsorbers, electrolytes and catalysts present in photoelectrochemical cells is essential. Here we review recent progress and open challenges in predicting physicochemical properties of heterogeneous interfaces for solar water splitting applications using first-principles-based approaches, and highlights the key role of these calculations in interpreting increasingly complex experiments.
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Accurate quantification of the stability of the perylene-tetracarboxylic dianhydride on Au(111) molecule–surface interface
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This work was supported by the NSF-CCI grant (CHE-1305124). Part of this work was performed under the auspices of the US Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. T.A.P. acknowledges support from the Lawrence Fellowship. We thank B. Wood, T. Ogitsu and E. Schwegler for useful discussions.
The authors declare no competing financial interests.
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Pham, T., Ping, Y. & Galli, G. Modelling heterogeneous interfaces for solar water splitting. Nature Mater 16, 401–408 (2017). https://doi.org/10.1038/nmat4803
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