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Isolating Cu-Zn active-sites in Ordered Intermetallics to Enhance Nitrite-to-Ammonia Electroreduction
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Journal Article
Isolating Cu-Zn active-sites in Ordered Intermetallics to Enhance Nitrite-to-Ammonia Electroreduction
2024
Overview
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 NH
3
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 NH
3
Faraday efficiency of ~80% and high NO
2
‒
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 *NO
2
and thus greatly facilitating the selective reduction of NO
2
−
into NH
3
.
Electrocatalytic nitrite reduction is a green alternative to the Haber-Bosch process, but its ammonia production remains inefficient at low nitrite levels. Here the authors report an intermetallic single atom alloy CuZn catalyst for nitrite reduction to ammonia with high efficiency and stability at low nitrite concentration of 1−10 mM.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
Subject
