Designing 2D carbon dot nanoreactors for alcohol oxidation coupled with hydrogen evolution
Qitao Chen, Baodong Mao, Yanhong Liu, Yunjie Zhou, Hui Huang, Song Wang, Longhua Li, Wei‐Cheng Yan, Weidong Shi, Zhenhui Kang
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. Cu-doped ZnIn2S4 nanosheets decorated with carbon dots are reported for the photocatalytic oxidation of organic alcohols coupled with H2 evolution with enhanced yields due to efficient charge accumulation and mass transfer at the catalyst surface.