![]() ![]() In principle, the C-C kinetics are dominated by two factors, the surface coverage of local adsorbed carbon monoxide (*CO) and the adsorption energy of *CO 12, 20, 21. These examples evidence the practicability of C 2+ production by such a cascade CO 2RR mechanism, which integrates two consecutive steps of CO 2-to-CO and CO-to-C 2+ on two distinct catalytic sites. Specifically, they prepared segmented tandem electrodes, where a CO-selective catalyst layer (CL) segment at the inlet prolongs the CO residence time in the subsequent C 2+ selective segment, resulting in a high C 2+ FE over the Cu/Fe-N-C catalysts. applied such a cascade catalysis to the design of gas diffusion electrodes (GDEs) 20. improved the C 2+ partial current over the Cu catalyst from 37 to 160 mA cm −2 by simply adding Ag nanoparticles to the catalyst, proving the effectiveness of cascade catalysis under industrial current densities 19. ![]() The CO 2 can be reduced into CO on the Ag core and then transferred to the Cu shell for further reduction into multicarbon products 18. ![]() put forward a cascade catalysis strategy to improve the multicarbon production with an core-shell structured catalyst 18. Inspired by the complex multistep cascade reactions in enzymes, O’Mara et al. Accordingly, various catalyst design strategies have been developed to improve the performance of multicarbon products produced using Cu-based catalysts, for instance, alloying, doping, surface modification, and interface engineering 14, 15, 16, 17. ![]() The sluggish C-C coupling kinetics over pure Cu surface severely hinders the mass production of multicarbon products 11, 12, 13. reported the production of multicarbon products (C 2H 4, C 2H 5OH, CH 3COOH, n-C 3H 7OH, etc.) on copper (Cu) in 1989, Cu has been demonstrated to be the only metal that can effectively catalyze CO 2 into multicarbon products 9, 10. Therefore, producing multicarbon products from CO 2RR seems much more attractive than C 1 products 8. However, the application of electrocatalytic CO 2RR technology is limited by the low values of the C 1 products 5, 6, 7. In the past few decades, enormous progress has been made in single-carbon product generation through electrocatalytic CO 2 reduction reaction (CO 2RR), especially for carbon monoxide and formic acid 3, 4. Density functional theory calculations further demonstrate that the high multicarbon product selectivity results from cooperation between AgCu single-atom alloys and Ag nanoparticles, wherein the Ag single-atom doping of Cu nanoparticles increases the adsorption energy of *CO on Cu sites due to the asymmetric bonding of the Cu atom to the adjacent Ag atom with a compressive strain.Įlectrocatalytic reduction of CO 2 into valuable chemicals using renewable electricity provides a sustainable route for CO 2 recycling and utilization, playing a critical role in realizing a carbon-neutral cycle 1, 2. As a result, a Faradaic efficiency (FE) of 94 ± 4% toward multicarbon products is achieved with the as-prepared AgCu single-atom and nanoparticle catalyst under ~720 mA cm −2 working current density at −0.65 V in a flow cell with alkaline electrolyte. In this paper, we report a cascade AgCu single-atom and nanoparticle electrocatalyst, in which Ag nanoparticles produce CO and AgCu single-atom alloys promote C-C coupling kinetics. However, the unsatisfactory catalytic selectivity for multicarbon products severely hinders the practical application of this technology. Electrocatalytic CO 2 reduction into value-added multicarbon products offers a means to close the anthropogenic carbon cycle using renewable electricity. ![]()
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