Computational Approaches to Materials Design for Enhanced Photocatalytic Activity

Abstract

Photocatalysis has attracted widespread attention as it can effectively utilize solar energy to solve the energy crisis and environmental pollution through, e.g., photocatalytic water splitting, nitrogen reduction reaction, and carbon dioxide reduction. Theoretical calculations play an important role in revealing microscopic mechanisms and designing high-performance photocatalysts. In this chapter, we focus on three aspects in photocatalysis: (1) light absorption; (2) photogenerated carrier separation and recombination; and (3) redox reaction. Latest advances of theoretical studies by first-principles calculations and non-adiabatic molecular dynamics simulations are expanded upon, including the manipulation of band edge positions, the design of Z-scheme heterostructures, tuning photogenerated carrier lifetimes and redox energy barriers. In addition, controlling methods for designing high-performance photocatalysts are discussed. Finally, challenges and prospects in theoretical studies of photocatalysis are discussed.