Efficient Plasma Electrocatalysis for High-Purity Solid Ammonium Chloride Synthesis

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Abstract Ammonia (NH3), an essential chemical in the contemporary world, is emerged as a promising carbon-free energy carrier. Herein, plasma-electrocatalytic synthesis of ammonia (PESA), by combining plasma N2 fixation (PNF) with electrochemical nitrate/nitrite (NOx−) reduction reaction (eNOxRR), is integrated with an ammonia capture system to achieve NH3 synthesis and its further conversion into high-purity solid NH4Cl. Accordingly, we report a spinel-structured CuCo2O4/Fe3O4 catalyst that significantly boosts the overall PESA process. In the PNF step, theoretical analysis reveals that N2 and O2 exhibit stronger adsorption and more facile dissociation on CuCo2O4/Fe3O4, accounting for the enhanced NOx− yield rate (297.0 mmol h−1). For eNOxRR, the catalyst delivers an NH3 yield rate of 322.5 mg h−1 cm−2 and a Faradaic efficiency (FE) of 98.6%. Theoretical analysis further indicates that the key intermediate NO2* binds strongly to the active site on CuCo2O4/Fe3O4, while the reduced energy barrier facilitates the NH3 formation. The integrated capture unit allows virtually 100% recovery of NH3 from the catholyte within 20 min, enabling direct formation of high‑purity solid NH4Cl. Overall, this work provides an efficient plasma-electrocatalytic route for the integrated synthesis, separation, and upgrading of nitrogen products from air and water.

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