Colloidal Single‐Layer Photocatalysts for Methanol‐Storable Solar H2 Fuel

Abstract Molecular surfactants are widely used to control low‐dimensional morphologies, including 2D nanomaterials in colloidal chemical synthesis, but it is still highly challenging to accurately control single‐layer growth for 2D materials. A scalable stacking‐hinderable strategy to not only enable exclusive single‐layer growth mode for transition metal dichalcogenides (TMDs) selectively sandwiched by surfactant molecules but also retain sandwiched single‐layer TMDs' photoredox activities is developed. The single‐layer growth mechanism is well explained by theoretical calculation. Three types of single‐layer TMDs, including MoS 2 , WS 2 , and ReS 2 , are successfully synthesized and demonstrated in solar H 2 fuel production from hydrogen‐stored liquid carrier—methanol. Such H 2 fuel production from single‐layer MoS 2 nanosheets is CO x ‐free and reliably workable under room temperature and normal pressure with the generation rate reaching ≈617 µmole g −1 h −1 and excellent photoredox endurability. This strategy opens up the feasible avenue to develop methanol‐storable solar H 2 fuel with facile chemical rebonding actualized by 2D single‐layer photocatalysts.