Au-Added CuS Hollow Spheres to Regulate the Strength and Active Area of N2 Adsorption Sites for Electrochemical NH3 Production

Abstract

Ammonia is a chemical compound in considerable global demand and plays a crucial role as an environmentally friendly energy carrier for hydrogen energy storage. The electrochemical nitrogen reduction reaction (eNRR) using copper sulfide catalysts is being extensively studied as an environmentally sustainable approach to the energy-intensive Haber？Bosch process for ammonia production. In this study, we aimed to prepare CuS hollow spheres modified with Au nanoparticles using an antisolvent crystallization-based method to be used as the catalysts for eNRR. During the addition of Au to the CuS catalysts, the nitrogen adsorption strength and surface area of the CuS catalysts are significantly regulated and expanded, leading to a noticeable enhancement in electrocatalytic performance for eNRR. Specifically, the ammonia production rate of 2.4 μmol cm？2 h or jNH3 = 0.2 mA cm？2 is achieved at a selectivity of 52% in neutral aqueous electrolyte, which is more than a 2-fold increase compared to the unmodified CuS catalyst. The findings of this study can contribute to the development of sustainable and environmentally friendly ammonia production in the future.