Sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 A cm−2

Wanru Liao, Jun Wang, Ganghai Ni, Kang Liu, Changxu Liu, Shanyong Chen, Qiyou Wang, Yingkang Chen, Tao Luo, Xiqing Wang, Yanqiu Wang, Wenzhang Li, Ting-Shan Chan, Chao Ma, Hongmei Li, Ying Liang, Weizhen Liu, Junwei Fu (), Beidou Xi () and Min Liu ()
Additional contact information
Wanru Liao: Central South University
Jun Wang: Central South University
Ganghai Ni: Central South University
Kang Liu: Central South University
Changxu Liu: University of Exeter
Shanyong Chen: Central South University
Qiyou Wang: Central South University
Yingkang Chen: Central South University
Tao Luo: Central South University
Xiqing Wang: Central South University
Yanqiu Wang: Central South University
Wenzhang Li: Central South University
Ting-Shan Chan: National Synchrotron Radiation Research Center
Chao Ma: Hunan University
Hongmei Li: Central South University
Ying Liang: Central South University of Forestry and Technology
Weizhen Liu: South China University of Technology
Junwei Fu: Central South University
Beidou Xi: Chinese Research Academy of Environmental Sciences
Min Liu: Central South University

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Nitrate (NO3‒) pollution poses significant threats to water quality and global nitrogen cycles. Alkaline electrocatalytic NO3‒ reduction reaction (NO3RR) emerges as an attractive route for enabling NO3‒ removal and sustainable ammonia (NH3) synthesis. However, it suffers from insufficient proton (H+) supply in high pH conditions, restricting NO3‒-to-NH3 activity. Herein, we propose a halogen-mediated H+ feeding strategy to enhance the alkaline NO3RR performance. Our platform achieves near-100% NH3 Faradaic efficiency (pH = 14) with a current density of 2 A cm–2 and enables an over 99% NO3–-to-NH3 conversion efficiency. We also convert NO3‒ to high-purity NH4Cl with near-unity efficiency, suggesting a practical approach to valorizing pollutants into valuable ammonia products. Theoretical simulations and in situ experiments reveal that Cl-coordination endows a shifted d-band center of Pd atoms to construct local H+-abundant environments, through arousing dangling O-H water dissociation and fast *H desorption, for *NO intermediate hydrogenation and finally effective NO3‒-to-NH3 conversion.

Date: 2024
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DOI: 10.1038/s41467-024-45534-2

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