Highly Accessible Electrocatalyst with <i>I</i><i>n Situ</i> Formed Copper-Cluster Active Sites for Enhanced Nitrate-to-Ammonia Conversion.
basic_science · Level V
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- Record sourced from PubMed, PMID 39844596.
- Also identified by DOI 10.1021/acsnano.4c14802.
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Abstract
Ammonia synthesis via nitrate electroreduction is more attractive and sustainable than the energy-extensive Haber-Bosch process and intrinsically sluggish nitrogen electroreduction. Herein, we have designed a single-site Cu catalyst on hierarchical nitrogen-doped carbon nanocage support (Cu<sub>1</sub>/hNCNC) for nitrate electroreduction, which achieves an ultrahigh ammonia yield rate (YR<sub>NH3</sub>) of 99.4 mol h<sup>-1</sup> g<sub>Cu</sub><sup>-1</sup> (2.30 mol h<sup>-1</sup> g<sub>cat.</sub><sup>-1</sup>) with ammonia Faradaic efficiency (FE<sub>NH3</sub>) of 99.3%, far beyond the most reported single-site catalysts on carbon-based supports. The combined <i>operando</i> characterization and theoretical studies indicate that the <i>in situ</i> formed Cu-cluster active sites are responsible for the high YR<sub>NH3</sub> and FE<sub>NH3</sub> due to the enhanced NO<sub>3</sub><sup>-</sup> adsorption and subsequent protonation on the unique Cu<sub>3</sub>-N<sub>4</sub> moieties, and meanwhile, the hierarchical hNCNC support facilitates the mass/charge transfer kinetics, thus promoting the high expression of intrinsic activity. The demonstration of plasma N<sub>2</sub> oxidization and nitrate electroreduction cascade reaction manifests the great potential of the Cu<sub>1</sub>/hNCNC electrocatalyst in sustainable NH<sub>3</sub> synthesis. These findings offer valuable insights into the design of effective catalysts for electrosynthetic reactions.