(ZnO)12 Cluster Decorated 2D Porous CN Materials as Efficient Solar Cells

Developing high-performance solar cells is a practical way to improve clean energy conversion efficiency. However, the performance of solar cells faces challenges such as fast carrier combination, poor stability, and limited solar light harvesting. Herein, we propose a strategy by decorating periodic holes in two-dimensional (2D) porous carbon–nitrogen (CN) materials with a zero-dimensional (0D) semiconducting (ZnO)₁₂ cluster. The effects of different CN substrates on the photogenerated carrier dynamics and solar cell performance are revealed by first-principles calculations combined with time-dependent ab initio nonadiabatic molecular dynamic (NAMD) simulations. With high structural stabilities, proper energy gaps of 1.81–3.23 eV, and positions, (ZnO)₁₂/CN heterostructures possess enhanced light absorption in the visible region, excellent separation of photogenerated electron–hole pairs with carrier relaxation times of 140–773 ns for electrons and 82–128 ns for holes, and large short-circuit current densities of 15–34 mA cm^–1. The study unveils the fundamental principles for optimizing the solar cell efficiency of metal oxide cluster decorated CN materials in energy conversion.