Rational Design of Two-Dimensional Binary Polymers from Heterotriangulenes for Photocatalytic Water Splitting

Abstract

On the basis of first-principles calculations, we report the design of three twodimensional (2D) binary honeycomb-kagome polymers composed of B-and N-centered heterotriangulenes with a periodically alternate arrangement as in hexagonal boron nitride. The 2D binary polymers with donor−acceptor characteristics are semiconductors with a direct band gap of 1.98−2.28 eV. The enhanced in-plane electron conjugation contributes to high charge carrier mobilities for both electrons and holes, about 6.70 and 0.24 × 10 3 cm 2 V −1 s −1 , respectively, for the 2D binary polymer with carbonyl bridges (2D CTPAB). With appropriate band edge alignment to match the water redox potentials and pronounced light adsorption for the ultraviolet and visible range of spectra, 2D CTPAB is predicted to be an effective photocatalyst/photoelectrocatalyst to promote overall water splitting.

β-SnS/GaSe heterostructure: a promising solar-driven photocatalyst with low carrier recombination for overall water splitting

“…Following the previous reports, 46–48 we finally calculate the Gibbs free energy profiles of the OER and HER involved in photocatalytic water splitting on the GaSe and β-SnS surfaces, respectively. Fig.…”

“…To address the photocatalytic water splitting, the Gibbs free energy profiles of the OER and HER processes on the GaSe and β-SnS surfaces, respectively, are calculated by adopting the method from previous reports, 46–48 see the ESI †…”

Thgraphene: a novel two-dimensional carbon allotrope as a potential multifunctional material for electrochemical water splitting and potassium-ion batteries

“…Recently, low-cost and noble metal-free HER and OER catalysts for overall water splitting have drawn more and more attention. [66][67][68] Considerable time and effort has been devoted to searching for abundant and high-efficiency electrocatalysts with low overpotential. Carbon-based materials have natural advantages from their structural diversity and are costeffective compared with metal-based materials.…”

Suppressing the Excitonic Effect in Covalent Organic Frameworks for Metal-Free Hydrogen Generation

“… 25 , 26 The unique attributes of COFs including high crystallinity, a tunable pore size, a large specific surface area, and high chemical and thermal stability make them promising candidates for photocatalysis. 27 − 32 Very recently, layer-stacked COFs with impressive hydrogen evolution activities have been reported, such as azine-linked N 3 -COF and cyano-vinylene-linked sp 2 c-COF, and it was shown that functionalization of sp 2 c-COF with electron-withdrawing end groups further increased the hydrogen production rate. 18 , 22 Despite the rapid experimental progress, 33 − 40 few studies reported an STH energy conversion efficiency of above 1%.…”