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Nanocluster-agminated amorphous cobalt nanofilms for highly selective electroreduction of nitrate to ammonia.
Jiang, Minghang; Zhu, Mengfei; Ding, Junjie; Wang, Huaizhu; Yu, Qianchuan; Chen, Xi; He, Yi; Wang, Mengjun; Luo, Xiaojun; Wu, Caijun; Zhang, Liyun; Yao, Xinghui; Wang, Huizhen; Li, Xiao; Liao, Xuemei; Jiang, Zhenju; Jin, Zhong.
Afiliação
  • Jiang M; Department of Chemistry, School of Science, Xihua University, Chengdu, Sichuan 610039, China; State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organi
  • Zhu M; State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Research Institute
  • Ding J; College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing 401331, China.
  • Wang H; State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Research Institute
  • Yu Q; State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Research Institute
  • Chen X; Department of Chemistry, School of Science, Xihua University, Chengdu, Sichuan 610039, China.
  • He Y; Department of Chemistry, School of Science, Xihua University, Chengdu, Sichuan 610039, China.
  • Wang M; Department of Chemistry, School of Science, Xihua University, Chengdu, Sichuan 610039, China.
  • Luo X; Department of Chemistry, School of Science, Xihua University, Chengdu, Sichuan 610039, China.
  • Wu C; Department of Chemistry, School of Science, Xihua University, Chengdu, Sichuan 610039, China.
  • Zhang L; Department of Chemistry, School of Science, Xihua University, Chengdu, Sichuan 610039, China.
  • Yao X; Department of Chemistry, School of Science, Xihua University, Chengdu, Sichuan 610039, China.
  • Wang H; Department of Chemistry, School of Science, Xihua University, Chengdu, Sichuan 610039, China.
  • Li X; College of Chemistry and Food Science, Yulin Normal University, Yulin, Guangxi 537000, China. Electronic address: leex211@126.com.
  • Liao X; Department of Chemistry, School of Science, Xihua University, Chengdu, Sichuan 610039, China; School of Food and Biological Engineering, Xihua University, Chengdu, Sichuan 610039, China. Electronic address: xmliao@mail.xhu.edu.cn.
  • Jiang Z; Department of Chemistry, School of Science, Xihua University, Chengdu, Sichuan 610039, China; School of Food and Biological Engineering, Xihua University, Chengdu, Sichuan 610039, China. Electronic address: zhjjiang@mail.xhu.edu.cn.
  • Jin Z; State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Research Institute
J Hazard Mater ; 476: 134909, 2024 Jun 18.
Article em En | MEDLINE | ID: mdl-38905979
ABSTRACT
Developing highly-efficient electrocatalysts for the nitrate reduction reaction (NITRR) is a persistent challenge. Here, we present the successful synthesis of 14 amorphous/low crystallinity metal nanofilms on three-dimensional carbon fibers (M-NFs/CP), including Al, Ti, Mn, Fe, Co, Ni, Cu, Zn, Ag, In, Sn, Pb, Au, or Bi, using rapid thermal evaporation. Among these samples, our study identifies the amorphous Co nanofilm with fine agglomerated Co clusters as the optimal electrocatalyst for NITRR in a neutral medium. The resulting Co-NFs/CP exhibits a remarkable Faradaic efficiency (FENH3) of 91.15 % at - 0.9 V vs RHE, surpassing commercial Co foil (39 %) and Co powder (20 %), despite sharing the same metal composition. Furthermore, during the electrochemical NITRR, the key intermediates on the surface of the Co-NFs/CP catalyst were detected by in situ Fourier-transform infrared (FTIR) spectroscopy, and the possible reaction ways were probed by Density functional theory (DFT) calculations. Theoretical calculations illustrate that the abundant low-coordinate Co atoms of Co-NFs/CP could enhances the adsorption of *NO3 intermediates compared to crystalline Co. Additionally, the amorphous Co structure lowers the energy barrier for the rate-determining step (*NH2→*NH3). This work opens a new avenue for the controllable synthesis of amorphous/low crystallinity metal nano-catalysts for various electrocatalysis reaction applications.
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Texto completo: 1 Bases de dados: MEDLINE Idioma: En Revista: J Hazard Mater Assunto da revista: SAUDE AMBIENTAL Ano de publicação: 2024 Tipo de documento: Article

Texto completo: 1 Bases de dados: MEDLINE Idioma: En Revista: J Hazard Mater Assunto da revista: SAUDE AMBIENTAL Ano de publicação: 2024 Tipo de documento: Article