Reconstructed Cu <sub>2</sub> O@CuCo Heterostructure with Accelerated Hydrogenation Kinetics for Air Plasma-Derived Ammonia Synthesis
Gaoming Jin, Pengzuo Chen, Yun Xiang Tong
Abstract
Ammonia (NH 3 ) is a key chemical for sustainable energy and nitrogen utilization, and air plasma-derived electrochemical NH 3 synthesis offers a promising alternative to traditional methods, yet significant challenges remain. Here, we develop an R-Cu 2 O@CuCo catalyst with abundant heterogeneous interfaces and strong electronic interactions via a facile chemical synthesis and electroreduction reconstruction strategy, exhibiting excellent NO 2 – -to-NH 3 performance. Benefiting from the efficient activation of active hydrogen intermediates by R-Cu 2 O@CuCo, NH 3 Faradaic efficiencies (FE) exceeding 90% are achieved over a wide voltage range (0 V vs RHE to −0.5 V vs RHE), with maximum FE and NH 3 yield reaching 95.4% at −0.1 V vs RHE and 1.22 mmol h –1 cm –2 at −0.6 V vs RHE, outperforming most reported catalysts. More importantly, a complete NH 3 synthesis system is realized by integrating spark discharge plasma for air-to-NO x – conversion and electrocatalytic reduction of NO x – -to-NH 3 using R-Cu 2 O@CuCo in a membrane electrode assembly (MEA) electrolyzer, enabling real-time NH 4 Cl product separation. Furthermore, demonstrating practical applicability, a Zn-NO 2 – battery achieves a high NH 3 production rate, maximum power density of 6.35 mW cm –2 and outstanding stability. This work paves the way for the development of advanced catalysts for continuous and efficient energy conversion systems.