Ionic covalent organic framework-MXene heterojunction constructed by electrostatic interaction for stable electrocatalytic hydrogen generation

Abstract

Constructing stable electrocatalysts by pyrolysis-free technique is an important topic in hydrogen-evolution reaction (HER) for water splitting reactions. Covalent organic frameworks (COFs), an emerging class of porous materials, offer ideal candidates owing to their abundant active sites and unique structures. Herein, a novel pyrolysis-free heterostructure was constructed using electrostatic interactions between an ionic COF (JUC-628) and Ti3C2Tx (MXene) nanosheets, which exhibits an impressively low overpotential of 137 mV at 10 mA cm−2 and excellent catalytic activity and stability for five days operation under alkaline conditions. Theoretical calculations depict that the formation of a stable heterostructure between MXene nanosheets and JUC-628 is the critical factor underlying the outstanding catalytic performance. Moreover, the optimized catalyst showed superior hydrogen-evolution capability in alkaline seawater electrolysis, highlighting the first successful application of a COF-based catalyst for hydrogen production from seawater electrolysis. As a leading covalent organic porous material–based catalyst for HER, as a proof of concept, this study represents a novel strategy to construct efficient electrocatalysts by COFs directly without the pyrolysis technique.