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Efficient and Selective Electrochemical Nitrate Reduction to N2 Using a Flow-Through Zero-Gap Electrochemical Reactor with a Reconstructed Cu(OH)2 Cathode: Insights into the Importance of Inter-Electrode Distance.
Zhou, Jianjun; Zhu, Yunqing; Wen, Kaiyue; Pan, Fan; Ma, Hongrui; Niu, Junfeng; Wang, Chuanyi; Zhao, Jincai.
Afiliación
  • Zhou J; School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xian 710021, China.
  • Zhu Y; College of Chemistry and Environmental Engineering, Yangtze University, Jingzhou 434023, China.
  • Wen K; School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xian 710021, China.
  • Pan F; School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xian 710021, China.
  • Ma H; School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xian 710021, China.
  • Niu J; School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xian 710021, China.
  • Wang C; College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, China.
  • Zhao J; School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xian 710021, China.
Environ Sci Technol ; 58(10): 4824-4836, 2024 Mar 12.
Article en En | MEDLINE | ID: mdl-38408018
ABSTRACT
Electrochemically converting nitrate, a widely distributed nitrogen contaminant, into harmless N2 is a feasible and environmentally friendly route to close the anthropogenic nitrogen-based cycle. However, it is currently hindered by sluggish kinetics and low N2 selectivity, as well as scarce attention to reactor configuration. Here, we report a flow-through zero-gap electrochemical reactor that shows a high performance of nitrate reduction with 100% conversion and 80.36% selectivity of desired N2 in the chlorine-free system at 100 mg-N·L-1 NO3- while maintaining a rapid reduction kinetics of 0.07676 min-1. More importantly, the mass transport and current utilization efficiency are significantly improved by shortening the inter-electrode distance, especially in the zero-gap electrocatalytic system where the current efficiency reached 50.15% at 5 mA·cm-2. Detailed characterizations demonstrated that during the electroreduction process, partial Cu(OH)2 on the cathode surface was reconstructed into stable Cu/Cu2O as the active phase for efficient nitrate reduction. In situ characterizations revealed that the highly selective *NO to *N conversion and the N-N coupling step played crucial roles during the selective reduction of NO3- to N2 in the zero-gap electrochemical system. In addition, theoretical calculations demonstrated that improving the key intermediate *N coverage could effectively facilitate the N-N coupling step, thereby promoting N2 selectivity. Moreover, the environmental and economic benefits and long-term stability shown by the treatment of real nitrate-containing wastewater make our proposed electrocatalytic system more attractive for practical applications.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Aguas Residuales / Nitratos Idioma: En Revista: Environ Sci Technol Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Aguas Residuales / Nitratos Idioma: En Revista: Environ Sci Technol Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Estados Unidos