Water Splitting with a Single-Atom Cu/TiO<sub>2</sub> Photocatalyst: Atomistic Origin of High Efficiency and Proposed Enhancement by Spin Selection
Cheng Cheng, Wei‐Hai Fang, Run Long, Oleg V. Prezhdo
Abstract
can be enhanced by spin selection, achievable experimentally via optical intersite spin transfer or chiral semiconductor coating. Both H adsorption and spin selection enhance charge carrier lifetimes by an order of magnitude. The spin selection mechanism does not require formation of the H species, which necessitates concurrent sources of electrons and protons and which is intrinsically unstable because water splitting involves frequent proton shuffling. Our results rationalize the experimental observations at the atomistic level, provide mechanistic insights into operation of single atom photocatalysis, and demonstrate that spin selection can be used to develop advanced and efficient systems for solar energy conversion.