Freestanding Hierarchical Carbon Nitride/Carbon-Paper Electrode as a Photoelectrocatalyst for Water Splitting and Dye Degradation

Freestanding electrodes composed of 2D materials are highly attractive for many applications such as batteries, membranes, actuators, optical devices, and other energy-related devices owing to their low price, unique structure, high specific surface area, and excellent mechanical and electrical properties. Here, we report the facile large-scale fabrication of freestanding hierarchical carbon nitride/carbon electrodes (CN/C) by the in situ crystallization of CN precursors on conductive carbon paper, followed by thermal annealing. The resulting CN exhibits a vertically aligned morphology with a homogeneous layer distribution, improved crystallinity, and excellent contact with the carbon paper. The freestanding electrodes exhibit high electrical conductivity and good photoelectrochemical activity as anodes in water splitting photoelectrochemical cells. Furthermore, we show here as a proof-of-concept that the freestanding CN/C electrodes can be used as photoelectrocatalysts for the oxidative degradation of organic compounds in water, with enhanced activity compared to photocatalytic and electrocatalytic degradation, while the extracted electrons can be used for the simultaneous production of hydrogen at the cathode.