Highly stabilized and selective ammonia electro‐oxidation over CuNi metallic glass nanoarray

Abstract Electrochemical nitrogen looping represents a promising carbon‐free and sustainable solution for the energy transition, in which electrochemical ammonia oxidation stays at the central position. However, the various nitrogen‐containing intermediates tend to poison and corrode the electrocatalysts, even the state‐of‐the‐art noble‐metal ones, which is worsened at a high applied potential. Herein, we present an ultrarapid laser quenching strategy for constructing a corrosion‐resistant and nanostructured CuNi alloy metallic glass electrocatalyst. In this material, single‐atom Cu species are firmly bonded with the surrounding Ni atoms, endowing exceptional resistance against ammonia corrosion relative of conventional CuNi alloys. Remarkably, a record‐high durability for over 300 h is achieved. Ultrarapid quenching also allows a much higher Cu content than typical single‐atom alloys, simultaneously yielding a high rate and selectivity for ammonia oxidation reaction (AOR). Consequently, an outstanding ammonia conversion rate of up to 95% is achieved with 91.8% selectivity toward nitrite after 8 h. Theoretical simulations reveal that the structural amorphization of CuNi alloy could effectively modify the electronic configuration and reaction pathway, generating stable single‐atom Cu active sites with low kinetic barriers for AOR. This ultrarapid laser quenching strategy thus provides a new avenue for constructing metallic glasses with well‐defined nanostructures, presenting feasible opportunities for performance enhancement for AOR and other electrocatalytic processes.