Spin-Selective Anti-Perovskite Enables Breakthrough Nitrate-to-Ammonia Electrocatalysis.
basic_science · Level V
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- Record sourced from PubMed, PMID 41684144.
- Also identified by DOI 10.1002/adma.202523066 and PMC identifier 12994318.
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Abstract
Electrochemical nitrate reduction to ammonia offers environmental and energy benefits, but progress is hindered by sluggish multistep proton-coupled electron transfers and competing side reactions. Here, we introduce an antiperovskite CuNCo<sub>3</sub> catalyst featuring a 3d-3d interaction framework. This framework stabilizes spin-selective Co sites even upon surface Co-N bond cleavage and drives asymmetric nitrate consumption. CuNCo<sub>3</sub> achieves 100% Faradaic efficiency and an NH<sub>3</sub> production rate of 124.6 mg mg<sub>cat</sub> <sup>-1</sup> h<sup>-1</sup> at -0.4 V vs. RHE. Operando XAS, XES, and ATR-FTIR directly link the evolution of spin-selective Co sites with specific NO<sub>3</sub>RR intermediates, revealing that spin-selective Co sites lower hydrogenation barriers and accelerate key steps. These results demonstrate that spin-selective anti-perovskite frameworks provide a robust, earth-abundant platform for high-performance nitrate-to-ammonia electrocatalysts.