Designing 2D carbon dot nanoreactors for alcohol oxidation coupled with hydrogen evolution

Abstract

The coupled green energy and chemical production by photocatalysis represents a promising sustainable pathway, which poses great challenges for the multifunction integration of catalytic systems. Here we show a promising green photocatalyst design using Cu-ZnIn₂S₄ nanosheets and carbon dots as building units, which enables the integration of reaction, mass transfer, and separation functions in the nano-space, mimicking a nanoreactor. This function integration results in great activity promotion for benzyl alcohol oxidation coupled H₂ production, with H₂/benzaldehyde production rates of 45.95/46.47 mmol g⁻¹ h⁻¹, 36.87 and 36.73 times to pure ZnIn₂S₄, respectively, owning to the enhanced charge accumulation and mass transfer according to in-situ spectroscopies and computational simulations of the built-in electrical field. Near-unity selectivity of benzaldehyde is achieved via the effective separation enabled by the Cu(II)-mediated conformation flipping of the intermediates and subsequent π-π conjugation. This work demonstrates an inspiring proof-of-concept nanoreactor design of photocatalysts for coupled sustainable systems.