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

Chen, Qitao; Mao, Baodong; Liu, Yanhong; Zhou, Yunjie; Huang, Hui; Wang, Song; Li, Longhua; Yan, Wei-Cheng et al. · Nat Commun · 2024

basic_science · Level V

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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-ZnIn<sub>2</sub>S<sub>4</sub> 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 H<sub>2</sub> production, with H<sub>2</sub>/benzaldehyde production rates of 45.95/46.47 mmol g<sup>-1</sup> h<sup>-1</sup>, 36.87 and 36.73 times to pure ZnIn<sub>2</sub>S<sub>4</sub>, 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.