摘要
Tremendous efforts have been devoted to explore energy-efficient strategies of ammonia synthesis to replace Haber-Bosch process which accounts for 1.4% of the annual energy consumption. In this study, atomically dispersed Au_1 catalyst is synthesized and applied in electrochemical synthesis of ammonia under ambient conditions. A high NH＋4 Faradaic efficiency of 11.1 % achieved by our Au_1 catalyst surpasses most of reported catalysts under comparable conditions. Benefiting from efficient atom utilization, an NH＋4 yield rate of 1,305 μg h-1 mg-1Au has been reached, which is roughly 22.5 times as high as that by sup- ported Au nanoparticles. We also demonstrate that by employing our Au_1 catalyst, NH＋4 can be electro- chemically produced directly from N_2 and H_2 with an energy utilization rate of 4.02 mmol kJ-1. Our study provides a possibility of replacing the Haber-Bosch process with environmentally benign and energy-efficient electrochemical strategies.
Tremendous efforts have been devoted to explore energy-efficient strategies of ammonia synthesis to replace Haber–Bosch process which accounts for 1.4% of the annual energy consumption. In this study,atomically dispersed Au_1 catalyst is synthesized and applied in electrochemical synthesis of ammonia under ambient conditions. A high NH_4^+ Faradaic efficiency of 11.1% achieved by our Au_1 catalyst surpasses most of reported catalysts under comparable conditions. Benefiting from efficient atom utilization, an NH_4^+ yield rate of 1,305 lg h^(-1) mg_(Au)^(-1) has been reached, which is roughly 22.5 times as high as that by supported Au nanoparticles. We also demonstrate that by employing our Au_1 catalyst, NH4+can be electrochemically produced directly from N_2 and H_2 with an energy utilization rate of 4.02 mmol kJ^(-1). Our study provides a possibility of replacing the Haber–Bosch process with environmentally benign and energy-efficient electrochemical strategies.
基金
supported by the National Key R&D Program of China (2017YFA0208300)
the National Natural Science Foundation of China (21522107, 21671180, 21521091, 21390393, U1463202, and 21522305)
作者简介
Xiaoqian Wang received his B.Sc. in materials physics in Jiaxi Lu Talent Program from University of Science and Technology of China in 2016. He is now pursing his Ph.D. degree under supervision of Prof. Yuen Wu at iChEM （Collaborative Innovation Center of Chemistry for Energy Materials）, University of Science and Technology of China. His current research interests focus on the application of nanomaterials in energy conversion and storage.;Yuen Wu received his B.Sc. and Ph.D. degrees from the Department of Chemistry, Tsinghua University in 2009 and 2014, respectively. He is currently a professor in the Department of Chemistry, University of Science and Technology of China. His research interests are focused on the synthesis, assembly, characterization and appli- cation of functional nanomaterials.
