Publication date: 11th July 2022
Photocatalytic water splitting is a promising solution to sustainable hydrogen production. Covalent organic frameworks (COFs) with highly designable skeleton and inherent pores have emerged as promising photocatalysts for water splitting. However, the strong excitonic effect and lack of active sites in COFs can impede the promotion of energy conversion efficiency. Here, we propose a facile approach to suppress the excitonic effect in COFs, which is by narrowing the band gap and increasing the dielectric screening. We precisely tailor the donor (D) and acceptor (A) building blocks of COFs of Lieb lattice, to simultaneously achieve visible light absorption, prompt exciton dissociation, and metal-free catalysis. Based on the GW-BSE method, we unravel a linear relationship between the electronic dielectric constant and the inverse square of the optical band gap of COFs of the Lieb lattice. We further demonstrate that both reduced exciton binding energy and enhanced sunlight absorption can be simultaneously realized in COFs with a narrow band gap. Specifically, we show that one of our designed COFs, PPy-TDQ whose exciton binding energy is nearly half that of g-C3N4 is capable of metal-free hydrogen production under near-infrared light irradiation. Our results present an effective method to suppress the excitonic effect in COFs and also pave the way for their applications in photocatalytic, photovoltaic, and other related solar energy conversions.
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