Computation-based regulation of excitonic effects in donor-acceptor covalent organic frameworks for enhanced photocatalysis

Abstract The strong excitonic effects widely exist in polymer-semiconductors and the large exciton binding energy ( E b ) seriously limits their photocatalysis. Herein, density functional theory (DFT) calculations are conducted to assess band alignment and charge transfer feature of potential donor-acceptor (D-A) covalent organic frameworks (COFs), using 1,3,5-tris(4-aminophenyl)triazine (TAPT) or 1,3,5-tris(4-aminophenyl)benzene (TAPB) as acceptors and tereph-thaldehydes functionalized diverse groups as donors. Given the discernable D-A interaction strengths in the D-A pairs, their E b can be systematically regulated with minimum E b in TAPT-OMe. Guided by these results, the corresponding D-A COFs are…

• NN
  National Natural Science Foundation of China

  Awards: U22A20401, 22161142001, U22A20401, 22161142001
• UO
  University of Science and Technology of China
• NK
  National Key Research and Development Program of China

  Award: 2021YFA1500400