Introducing Spin Polarization into Mixed-Dimensional Van der Waals Heterostructures for High-Efficiency Visible-Light Photocatalysis

The low separation efficiency of the photogenerated carrier and the poor activity of the surface redox reaction are the main barrier to further improvement of photocatalytic materials. To address these issues, introducing spin-polarized electrons in single-component photocatalytic materials emerged as a promising approach. However, the decreased redox ability of photocarriers in these materials becomes a new challenge. Herein, we mitigate this challenge with a carbon nitride sheet (CNs)/graphene nanoribbon (GNR) composite material that has a van der Waals heterostructures (vdWHs) and spin-polarized electron properties. Experimental results and theoretical calculations show that the heterostructure has a strong redox ability, high carrier-separation efficiency, and enhanced surface catalytic reaction. Consequently, the mixed-dimensional CNs/GNR vdWHs exhibit remarkable performance for H₂ and O₂ generation as well as CO₂ production under visible-light irradiation without any cocatalyst. The spin-polarized vdWHs discovered in this study revealed a new type of photocatalytic materials and advanced the development of spintronics and photocatalysis.