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.

从水和阳光中产生氢为生产可扩展且可持续的无碳能源提供了一种有前途的方法。成功的太阳能燃料技术的关键是设计高效，持久且低成本的光电化学电池，该电池负责吸收阳光并推动水分解反应。为此，对光电化学电池中存在的光吸收剂，电解质和催化剂之间的异质界面的详细理解和控制是必不可少的。在这里，我们回顾了使用基于第一原理的方法在预测太阳能分水应用的非均质界面的理化特性方面的最新进展和面临的挑战，并强调了这些计算在解释日益复杂的实验中的关键作用。