P-Block Antimony-Copper Single-Atom Alloys for Selective Nitrite Electroreduction to Ammonia.
basic_science · Level V
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- Record sourced from PubMed, PMID 38718265.
- Also identified by DOI 10.1021/acsnano.4c01958.
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Abstract
Electrocatalytic reduction of NO<sub>2</sub><sup>-</sup> to NH<sub>3</sub> (NO<sub>2</sub>RR) offers an effective method for alleviating NO<sub>2</sub><sup>-</sup> pollution and generating valuable NH<sub>3</sub>. Herein, a p-block single-atom alloy, namely, isolated Sb alloyed in a Cu substrate (Sb<sub>1</sub>Cu), is explored as a durable and high-current-density NO<sub>2</sub>RR catalyst. As revealed by the theoretical calculations and operando spectroscopic measurements, we demonstrate that Sb<sub>1</sub> incorporation can not only hamper the competing hydrogen evolution reaction but also optimize the d-band center of Sb<sub>1</sub>Cu and intermediate adsorption energies to boost the protonation energetics of NO<sub>2</sub><sup>-</sup>-to-NH<sub>3</sub> conversion. Consequently, Sb<sub>1</sub>Cu integrated in a flow cell achieves an outstanding NH<sub>3</sub> yield rate of 2529.4 μmol h<sup>-1</sup> cm<sup>-2</sup> and FE<sub>NH3</sub> of 95.9% at a high current density of 424.2 mA cm<sup>-2</sup>, as well as a high durability for 100 h of electrolysis.