Modulating Hydrogen Species for Efficient and Sustainable Nitrate Electroreduction to Ammonia
Abstract
ABSTRACT The electrochemical nitrate reduction reaction (NO 3 RR) represents a promising strategy for sustainable NH 3 synthesis and environmental remediation. However, developing an NH 3 production process that achieves both high current density and Faradaic efficiency (FE) is challenging owing to the strong electrostatic repulsion of NO 3 − from the electrode surface and the competing hydrogen evolution reaction at high current densities. Here, Cu/C electrode, modified using 1‐dodecanol (C 12 OH), achieves an exceptional NH 3 yield rate of 4.50 mmol cm −2 h −1 and FE NH3 of 98.9% at 1.0 A cm −2 . This performance significantly surpasses that of the pristine Cu/C catalyst and most reported state‐of‐the‐art catalysts. C 12 OH modification, which induces the reconstruction of the hydrogen‐bonded network on the electrode surface, not only enhances NO 3 − enrichment but also promotes H • radical generation. This new pathway, mediated by H • radicals, is both thermodynamically and kinetically favorable and underlies the promoted NH 3 production.
Article Details
Authors (17)
Yiyong Wang
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Yingying Cheng
Mingxin Gao
Shiqiang Liu
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Huisheng Qin
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Wenling Zhao
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Xing Tong
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Xueqing Xing
Beijing Synchrotron Radiation Facility
Lihong Jing
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Pei Zhang
Department of Neurobiology, School of Basic Medicine, Tongji Medical College, Huazhong University of Science and Technology
Qinggong Zhu
Institute of Chemistry, Chinese Academy of Sciences , , ,
Xiaofu Sun
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Jianling Zhang
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Zhimin Liu
Yi Xu
Xinchen Kang
Institute of Chemistry, Chinese Academy of Sciences , , ,
Buxing Han
Institute of Chemistry, Chinese Academy of Sciences , , ,