Efficient Ambient Electrocatalytic Ammonia Synthesis by Nanogold Triggered via Boron Clusters Combined with Carbon Nanotubes

Currently, the development of stable electrochemical nitrogen reduction reaction (ENRR) catalysts with high N-2 conversion activity and low cost to instead of the traditional Haber-Bosch ammonia production process of high-energy consumption remains a great challenge for researchers. Here, we have immobilized reductive closo-[B12H11](-) boron clusters on a carbon nanotubes (CNT) surface and have successfully prepared a novel Au-CNT catalyst with extraordinary ENRR activity after adding HAuCl4 to the CNT-[B12H11](-) precursor. The excellent properties of ammonia yield (57.7 mu g h(-1) cm(-2)) and Faradaic efficiency (11.97%) make it possible to achieve using this Au-CNT catalyst in large-scale industrial production of ammonia. Furthermore, its outstanding cyclic stability and long-term tolerability performance make it one of the most cost-effective catalysts to date. Here, by means of density functional theory we disclose the associative mechanism of N-2-to-NH3 conversion on the Au(111) surface, providing visual theoretical support for the experimental results.