Efficient conversion of CO2 to accelerate the carbon cycle plays an essential role in the proposed goal for peaking carbon dioxide emissions before 2030. Electrochemical CO2 reduction reaction (ECR) is an effective strategy to convert CO2 into high-value fuels. Multi-carbon fuels are the essential raw materials in the chemical industry that generally need more electrons to reduce CO2 in ECR. Copper-based nanocatalysts have been proved to be the only catalyst that can produce multi-carbon fuels. However, copper-based catalysts have many mechanisms that reduce CO2 to multi-carbon products. Here, we synthesize a single Pd atom dispersed copper nitride (Cu3N) nanocube catalyst that possesses an antiperovskite-type structure. Cause of the lack of A-sites in copper nitride, Pd atoms could singly be dispersed in the Cu3N. As for the ECR performance, the faraday efficiency (FE) of multi-carbon products of Pd single-atomic site Cu3N (Pd-SAs/Cu3N) could be prominently increased to 56.2% compared to the bare Cu3N nanocubes (below 5.6%). Combining DFT calculation and operando characterization of XAFS, we come up with an ultralow coordination numbers copper intermediate could form in the reduction potential. Under normal conditions, the (100) facet of Cu3N is averse to the C-C coupling process for producing multi-carbon products. Singlet Pd atoms on the (100) facet could also have higher reactivity for C-C coupling and multi-carbon product production.

Single-atom Pd optimized copper nitride defects selectively reduce carbon dioxide electrochemically to multi-carbon products

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ACS Fall 2022

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.