Planar semiconductor junctions with robust driving forces synergistically orienting direct water splitting

Abstract

Pure water splitting by charged semiconductors and solar photons to concurrently generate H2 and O2 molecules has gained notable attention due to worldwide clean energy generation and storage. Despite significant advancements, challenges facing severe carrier recombination and sluggish electron transport continue to hinder the intrinsic efficiency of water splitting. Here, we fabricate two-dimensional graphitic carbon nitride-hybridized sulfur thionic polymorphs (CN/S100/S010 junctions) by incorporating photoactive semiconductors within lateral nanosheets. As a result, the charge rectification effect within the coplanar graphitic carbon nitride/S100/S010 junctions is induced by well-designed driving forces: favorable band offsets and cascade polarized surface work functions. During the water splitting process, the photogenerated electrons are sequentially transferred from graphitic carbon nitride to element semiconductor sulfur {100} and subsequently oriented to sulfur {010} facets. This unique behavior of charge migration within CN/S100/S010 photocatalysts contributes to impressive rates of H2 and O2 production, reaching 740 and 363 µmol g−1·h−1, respectively, nearly 13-fold higher than that of the parent carbon nitride. Comprehensive spectroscopic and theoretical analyses confirm the formation of CN/S100/S010 hierarchies with long-lived charge carriers during hydrogen energy production. This work introduces novel avenues for automatically orienting photogenerated carriers and holds promising prospects for clean energy production.