A coating strategy to achieve effective local charge separation for photocatalytic coevolution

Significance Particulate photocatalysis is a promising approach to solar fuels production at scale. Herein, we present a general design by using conformal coatings and attaching nanoscale cocatalysts to achieve local charge separation and, at the same time, to stabilize photocatalysts that are easily photocorroded otherwise. With spatial charge separation, the nanometer-spaced reductive and oxidative surface sites can coevolve to produce H2 and O2 , or to produce H2 and oxidize redox mediators, or to produce O2 and reduce redox mediators. This work investigates the charge separation strategy for the semiconductor/coating/cocatalyst structure both by tuning barrier height energetics and by building numerical models.