Isolating Cu-Zn active-sites in Ordered Intermetallics to Enhance Nitrite-to-Ammonia Electroreduction

Jiao Lan, Zhen Wang, Cheng-wei Kao, Ying-Rui Lu, Feng Xie and Yongwen Tan ()
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Jiao Lan: Hunan University
Zhen Wang: Hunan University
Cheng-wei Kao: National Synchrotron Radiation Research Center
Ying-Rui Lu: National Synchrotron Radiation Research Center
Feng Xie: Hunan University
Yongwen Tan: Hunan University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Electrocatalytic nitrite reduction to the valuable ammonia is a green and sustainable alternative to the conventional Haber-Bosch method for ammonia synthesis, while the activity and selectivity for ammonia production remains poor at low nitrite concentrations. Herein, we report a nanoporous intermetallic single-atom alloy CuZn (np/ISAA-CuZn) catalyst with completely isolated Cu-Zn active-sites, which achieves neutral nitrite reduction reaction with a remarkable NH3 Faradaic efficiency over 95% and the highest energy efficiency of ≈ 59.1% in wide potential range from −0.2 to −0.8 V vs. RHE. The np/ISAA-CuZn electrocatalyst was able to operate stably at 500 mA cm−2 for 220 h under membrane electrode assembly conditions with a stabilized NH3 Faraday efficiency of ~80% and high NO2‒ removal rate of ~100%. A series of in situ experimental studies combined with density functional theory calculations reveal that strong electronic interactions of isolated Cu-Zn active-sites altered the protonation adsorption species, effectively alleviating the protonation barrier of *NO2 and thus greatly facilitating the selective reduction of NO2− into NH3.

Date: 2024
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DOI: 10.1038/s41467-024-53897-9

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