Decoupling Interlayer Interactions Boosts Charge Separation in Covalent Organic Frameworks for High‐Efficiency Photocatalytic CO 2 Reduction

Abstract Covalent organic frameworks (COFs) have emerged as promising photocatalysts owing to their structural diversity, tunable bandgaps, and exceptional light‐harvesting capabilities. While previous studies primarily focus on developing narrow‐bandgap COFs for broad‐spectrum solar energy utilization, the critical role of interlayer coupling in regulating charge transfer dynamics remains unclear. Conventional monolayer‐based theoretical models inadequately address interlayer effects that potentially hindering intralayer electron transport to catalytic active sites. This work employs density functional theory (DFT) calculations to investigate the influence of interlayer interactions on intralayer charge…

• NN
  National Natural Science Foundation of China

  Awards: No. 22279143, 22279143