Semiconductor-based photocatalysis as a productive technology furnishes a prospective solution to environmental and renewable energy issues, but its efficiency greatly relies on the effective bulk and surface separation of photoexcited charge carriers. Exploitation of atomic-level strategies allows in-depth understanding on the related mechanisms and enables bottom-up precise design of photocatalysts, significantly enhancing photocatalytic activity. Herein, the advances on atomic-level charge separation strategies toward developing robust photocatalysts are highlighted, elucidating the fundamentals of charge separation and transfer processes and advanced probing techniques. The atomic-level bulk charge separation strategies, embodied by regulation of charge movement pathway and migration dynamic, boil down to shortening the charge diffusion distance to the atomic-scale, establishing atomic-level charge transfer channels, and enhancing the charge separation driving force. Meanwhile, regulating the in-plane surface structure and spatial surface structure are summarized as atomic-level surface charge separation strategies. Moreover, collaborative strategies for simultaneous manipulation of bulk and surface photocharges are also introduced. Finally, the existing challenges and future prospects for fabrication of state-of-the-art photocatalysts are discussed on the basis of a thorough comprehension of atomic-level charge separation strategies.
Keywords: atomic-level strategies; bulk charge separation; charge kinetics; photocatalysis; surface charge separation.
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