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

Yunyang Qian, Yulan Han, Xiyuan Zhang, Ge Yang, Guozhen Zhang and Hai-Long Jiang ()
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Yunyang Qian: University of Science and Technology of China
Yulan Han: University of Science and Technology of China
Xiyuan Zhang: University of Science and Technology of China
Ge Yang: University of Science and Technology of China
Guozhen Zhang: University of Science and Technology of China
Hai-Long Jiang: University of Science and Technology of China

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract The strong excitonic effects widely exist in polymer-semiconductors and the large exciton binding energy (Eb) 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 Eb can be systematically regulated with minimum Eb in TAPT-OMe. Guided by these results, the corresponding D-A COFs are synthesized, where TAPT-OMe-COF possesses the best activity in photocatalytic H2 production and the activity trend of other COFs is associated with that of calculated Eb for the D-A pairs. In addition, further alkyne cycloaddition for the imine linkage in the COFs greatly improves the stability and the resulting TAPT-OMe-alkyne-COF with a substantially smaller Eb exhibits ~20 times higher activity than the parent COF.

Date: 2023
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DOI: 10.1038/s41467-023-38884-w

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