Pulsed Electrocatalysis Driven Efficient Ammonia Synthesis by Facilitating *NOOH Formation and Balancing *H Supply
Abstract
Abstract Electrochemical nitrate reduction emerges as a promising approach for ammonia generation; however, its efficiency is hindered by the sluggish hydrogenation of nitrogen‐containing intermediates and limited active hydrogen supply at constant applied potentials. Driven by the pulsed electrocatalysis, in this work, efficient nitrate‐to‐ammonia conversion is realized by facilitating *NOOH formation and balancing *H supply on a Janus Cu@Co/NC electrocatalyst. In detail, the Cu sites could activate NO 3 − at low overpotentials, while the Co sites could facilitate *NOOH formation with sufficient *H provided by the Co sites at high overpotentials. Promoted by the pulsed electrocatalysis technique, a maximum Faradaic efficiency of 98.32% with NH 3 yield rate of 12.75 mg h −1 mg cat −1 is attained, and the scaled‐up pulsed electrosynthesis at industrial current densities is also achieved. This work underlines the feasibility of pulsed electrolysis for regulating intermediate hydrogenation, offering a promising approach for the synthesis of ammonia or other important chemicals.
Article Details
Authors (14)
Zeyu Li
Beijing National Laboratory for Molecular Sciences
Zichen Shi
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, State Key Laboratory of Space Power‐Sources School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin 150001 P.R. China
Yinggang Ou
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, State Key Laboratory of Space Power‐Sources School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin 150001 P.R. China
Lixiang Zhong
School of Physics, Beijing Institute of Technology 1 , Beijing, 100081,
Chunshuang Yan
Chu Zhang
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering
Kai Song
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Organic Solids, Institute of Chemistry
Hengjie Liu
National Synchrotron Radiation Laboratory, State Key Laboratory of Precision and Intelligent Chemistry
Daobin Liu
State Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, School of Chemistry and Materials Science
Pin Song
Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Engineering Research Center of Carbon Neutrality, College of Chemistry and Materials Science
Chenhui Yin
Zeming Qi
Li Song
Chade Lv
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering