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Single-atom catalysts have exhibited great potential in the photocatalytic conversion of CO2 to C2 products, but generation of gaseous multi-carbon hydrocarbon products is still challenging. Previously, supports of a single atom consist of multiple elements, making C-C coupling difficult because the coordination environment of single-atom sites is diversified and difficult to control. Here, we steer C-C coupling by implanting an Au single atom on the red phosphorus (Au1/RP), support with uniform structure composed of a single element, lower electronegativity, and better ability to absorb CO2. The electron-rich phosphorus atoms near the Au single atoms can function as active sites for CO2 activation. The Au single atom can effectively reduce the energy barrier of C-C coupling, boosting the reaction kinetics of the formation of C2H6. Notably, the C2H6 selectivity and turnover frequency of Au1/RP reach 96% and 7.39 h-1 without a sacrificial agent, respectively, which almost represents the best photocatalyst for C2 chemical synthesis to date. This research will provide new ideas for the design of high-efficiency photocatalysts for CO2 conversion to C2 products.
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Honghui Ou
State Key Laboratory of Hydrology-Water Resources and Hydraulic Engineering
Guosheng Li
Zhongyuan University of Technology
Wei Ren
Fujian Normal University
Journal of the American Chemical Society
Tsinghua University
Sun Yat-sen University
Beijing Normal University
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Ou et al. (Tue,) studied this question.
synapsesocial.com/papers/69d7dbf0a2a48916bbbee246 — DOI: https://doi.org/10.1021/jacs.2c09424