Understanding the Activity Trends in Electrocatalytic Nitrate Reduction to Ammonia on Cu Catalysts.
basic_science · Level V
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- Record sourced from PubMed, PMID 38071625.
- Also identified by DOI 10.1021/acs.nanolett.3c03962.
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Abstract
Cu-based catalysts possess great potential in the electrocatalytic nitrate (NO<sub>3</sub><sup>-</sup>) reduction reaction for ammonia (NH<sub>3</sub>) synthesis. However, the low atomic economy limits their further application. Here we report a Cu single-atom (SA) incorporated in nitrogen-doped carbon (Cu SA/NC) with high atomic economy, which exhibits superior NH<sub>3</sub> Faradaic efficiency (FE) of 100% along with an impressive NH<sub>3</sub> yield rate of 7480 μg h<sup>-1</sup> mg<sub>cat.</sub><sup>-1</sup>. As counterparts, Cu<sub>s+n</sub>/NC, with mixed SA and nanoparticles (NPs), shows decreasing NH<sub>3</sub> FE with decreasing SA content, but the production of N<sub>2</sub> and N<sub>2</sub>O increases gradually, which reaches the maximum on pure Cu NPs. In situ characterizations and theoretical calculations reveal that a higher NH<sub>3</sub> FE of Cu SA/NC is ascribed to a lower free energy of the rate-limiting step (HNO* → N*) and effective inhibition for the N-N coupled process. This work provides the intuitive activity trends of Cu-based catalysts, opening an avenue for subsequent catalysts design.