Industrial-current Ammonia Synthesis by Polarized Cuprous Cyanamide Coupled to Valorization of Glycerol at 4,000 mA cm<sup>−2</sup>School of Environmental Science and Technology, Dalian University of Technology, Dalian, 116024, China.
The State Key Laboratory of High-Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, China; Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China.
The State Key Laboratory of High-Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, China; Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China.
The State Key Laboratory of High-Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, China; Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China.
Department of Chemistry, Western University, 1151 Richmond Street, London, ON, N6A5B7, Canada, 1151 Richmond Street.
Department of Chemistry, Western University, 1151 Richmond Street, London, ON, N6A5B7, Canada, 1151 Richmond Street.
Department of Materials Design and Innovation, University at Buffalo, The State University of New York, Buffalo, NY, 14260, USA.
The State Key Laboratory of High-Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, China.
School of Environmental Science and Technology, Dalian University of Technology, Dalian, 116024, China.
The State Key Laboratory of High-Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, China; State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China.
The State Key Laboratory of High-Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, China; Zhejiang Key Laboratory for Island Green Energy and New Materials, Institute of Electrochemistry, School of Materials Science and Engineering, Taizhou University, Taizhou, 318000, China; Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071, China.
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2025 (English)In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 37, no 14, article id 2418451Article in journal (Refereed) Published
Abstract [en]
The electrocatalytic nitrate reduction (NO3RR) holds significance in both NH3 synthesis and nitrate contamination remediation. However, achieving industrial-scale current and high stability in membrane electrode assembly (MEA) electrolyzer remains challenging due to inherent high full-cell voltage for sluggish NO3RR and water oxidation. Here, Cu2NCN with positive surface electrostatic potential VS(r) is applied as highly efficient NO3RR electrocatalysts to achieve industrial-current and low-voltage stable NH3 production in MEA electrolyzer with coupled anodic glycerol oxidation. This paired electro-refinery (PER) system reaches 4000 mA cm−2 at 2.52 V and remains stable at industrial-level 1000 mA cm−2 for 100 h with the NH3 production rate of 97000 µgNH3 h−1 cm−2 and a Faradaic efficiency of 83%. Theoretical calculations elucidate that the asymmetric and electron-withdrawing [N−C≡N] units enhance polarization and VS(r), promoting robust and asymmetric adsorption of NO3* on Cu2NCN to facilitate O−N bond dissociation. A comprehensive techno-economic analysis demonstrates the profitability and commercial viability of this coupled system. Our work opens a new avenue and marks a significant advancement in MEA systems for industrial NH3 synthesis.
Place, publisher, year, edition, pages
Wiley , 2025. Vol. 37, no 14, article id 2418451
Keywords [en]
ammonia synthesis, nitrate reduction, paired electro-refinery system, surface electrostatic potential, techno-economic analysis
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-362538DOI: 10.1002/adma.202418451ISI: 001427003500001PubMedID: 39981855Scopus ID: 2-s2.0-85218705780OAI: oai:DiVA.org:kth-362538DiVA, id: diva2:1952986
Note
QC 20250422
2025-04-162025-04-162025-04-22Bibliographically approved