Ultrafast Interlayer Charge Separation, Enhanced Visible-Light Absorption, and Tunable Overpotential in Twisted Graphitic Carbon Nitride Bilayers for Water Splitting.

Moiré pattern superlattice formed by 2D van der Waals layered structures have attracted great attention for diverse applications. In experiments, the enhancement of catalytic performance in twisted bilayer systems is reported while its mechanism remains unclear. From high-accuracy first-principles and time-dependent ab initio nonadiabatic molecular dynamics calculations, ultrafast interlayer charge transfer within 120 fs, excellent charge separation, improved visible-light absorption, and satisfactory overpotentials for the hydrogen evolution and oxygen evolution reactions in twisted graphitic carbon nitride (g-C3 N4 ) bilayers are found, which are beneficial to photocatalytic, photo-electrocatalytic, or electrocatalytic water splitting. This work provides insightful guidance to advanced nanocatalysis based on twisted layered materials.