Abstract
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.
| Original language | English |
|---|---|
| Pages (from-to) | 22075-22082 |
| Number of pages | 8 |
| Journal | Journal of the American Chemical Society |
| Volume | 144 |
| Issue number | 48 |
| DOIs | |
| State | Published - 7 Dec 2022 |
| Externally published | Yes |
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