Ammonia(NH3)production via the electrochemical nitrogen reduction reaction(NRR)is a promising method for sustainable generation of this important chemical.Efforts are ongoing in finding an efficient,stable,and selecti...Ammonia(NH3)production via the electrochemical nitrogen reduction reaction(NRR)is a promising method for sustainable generation of this important chemical.Efforts are ongoing in finding an efficient,stable,and selective catalyst that will enable the reaction.However,progress is hindered in the field due to lack of reproducibility,most likely a consequence of reports of false-positive results due to improper measurement control and methods.In this study,we explore the NRR activity of a promising class of single atom catalysts,transition metal-nitrogen-carbon(M-N-C)electrocatalysts.Using a state-of-the-art in-line ammonia quantification methodology,with detection limit as low as 1 ppb for ammonia,we show that single atom Nb and Fe embedded in a stable carbon and nitrogen framework do not electrochemically reduce N_(2) to NH_(3).Critically,this demonstrates that our experimental setup with in-line sequential injection analysis successfully excludes ammonia contamination from the gas supply and atmospheric sources,allowing for thorough and high-throughput examination of potential NRR catalysts.展开更多
基金Atmonia and the University of Iceland would like to acknowledge the Icelandic Research Fund(grant 196437-051)the Icelandic Technology Development Fund(grant 175350-0611)for the financial support of this work.ABG gratefully acknowledges financial support from the Icelandic Research Fund(grant 1515-1513377).AS and BZ gratefully acknowledge the financial support from the U.S.Department of Energy's Office of Energy Efficiency and Renewable Energy(EERE)under the Hydrogen and Fuel Cells Technologies Office(HFTO),FY2018 Hydrogen and Fuel Cell R&D FOA,Award Number DE-EE0008419,and support from Companhia Brasileira de Metalurgia e Mineração(CBMM).
文摘Ammonia(NH3)production via the electrochemical nitrogen reduction reaction(NRR)is a promising method for sustainable generation of this important chemical.Efforts are ongoing in finding an efficient,stable,and selective catalyst that will enable the reaction.However,progress is hindered in the field due to lack of reproducibility,most likely a consequence of reports of false-positive results due to improper measurement control and methods.In this study,we explore the NRR activity of a promising class of single atom catalysts,transition metal-nitrogen-carbon(M-N-C)electrocatalysts.Using a state-of-the-art in-line ammonia quantification methodology,with detection limit as low as 1 ppb for ammonia,we show that single atom Nb and Fe embedded in a stable carbon and nitrogen framework do not electrochemically reduce N_(2) to NH_(3).Critically,this demonstrates that our experimental setup with in-line sequential injection analysis successfully excludes ammonia contamination from the gas supply and atmospheric sources,allowing for thorough and high-throughput examination of potential NRR catalysts.
