Hierarchically Porous Few-Layer Carbon Nitride and Its High H⁺ Selectivity for Efficient Photocatalytic Seawater Splitting

Abstract

Photocatalysts for seawater splitting are severely restricted because of the presence of multiple types of ions in seawater that cause corrosion and deactivation. As a result, new materials that promote adsorption of H⁺ and hinder competing adsorption of metal cations should enhance utilization of photogenerated electrons on the catalyst surface for efficient H₂ production. One strategy to design advanced photocatalysts involves introduction of hierarchical porous structures that enable fast mass transfer and creation of defect sites that promote selective hydrogen ion adsorption. Herein, we used a facile calcination method to fabricate the macro-mesoporous C₃N₄ derivative, V_N-HCN, that contains multiple nitrogen vacancies. We demonstrated that V_N-HCN has enhanced corrosion resistance and elevated photocatalytic H₂ production performance in seawater. Experimental results and theoretical calculations reveal that enhanced mass and carrier transfer and selective adsorption of hydrogen ions are key features of V_N-HCN that lead to its high seawater splitting activity.