Nanocarbon-Enhanced 2D Photoelectrodes: A New Paradigm in Photoelectrochemical Water Splitting

Abstract Solar-driven photoelectrochemical (PEC) water splitting systems are highly promising for converting solar energy into clean and sustainable chemical energy. In such PEC systems, an integrated photoelectrode incorporates a light harvester for absorbing solar energy, an interlayer for transporting photogenerated charge carriers, and a co-catalyst for triggering redox reactions. Thus, understanding the correlations between the intrinsic structural properties and functions of the photoelectrodes is crucial. Here we critically examine various 2D layered photoanodes/photocathodes, including graphitic carbon nitrides, transition metal dichalcogenides, layered double hydroxides, layered bismuth oxyhalide nanosheets, and MXenes, combined with advanced nanocarbons (carbon dots, carbon nanotubes, graphene, and graphdiyne) as co-catalysts to assemble integrated photoelectrodes for oxygen evolution/hydrogen evolution reactions. The fundamental principles of PEC water splitting and physicochemical properties of photoelectrodes and the associated catalytic reactions are analyzed. Elaborate strategies for the assembly of 2D photoelectrodes with nanocarbons to enhance the PEC performances are introduced. The mechanisms of interplay of 2D photoelectrodes and nanocarbon co-catalysts are further discussed. The challenges and opportunities in the field are identified to guide future research for maximizing the conversion efficiency of PEC water splitting.