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author:

Lan, Yi-Ying (Lan, Yi-Ying.) [1] | Chen, Wei-Xuan (Chen, Wei-Xuan.) [2] | Si, Duan-Hui (Si, Duan-Hui.) [3] | Zhu, Hong-Jing (Zhu, Hong-Jing.) [4] | Fu, Xiao-Xue (Fu, Xiao-Xue.) [5] | Huang, Yuan-Biao (Huang, Yuan-Biao.) [6] | Cao, Rong (Cao, Rong.) [7]

Abstract:

The electrocatalytic conversion of nitrate (NO3-) into ammonia (NH3) is an eco-friendly alternative approach that integrates eliminating the NO3-pollutants from water with the production of valueadded NH3. However, traditional working electrodes for the electrocatalytic NO3-reduction reaction (NO3RR) are primarily fabricated using binder-mediated techniques, which often result in low current densities due to the restricted electronic transport from the external voltage to the active sites. Herein, we develop a self-supporting electrode technique based on copper-based metal-organic framework (MOF) glasses for efficient electrocatalytic NO3RR towards NH3. The preparation of the copper-based MOF glass self-supporting electrode, denoted as agCu(MeIm)2-CC (where "a", "g", HMeIm and CC represent amorphous, glass, 2-methylimidazole, and carbon cloth, respectively) involves the ball-milling of crystalline Cu(MeIm)2 onto the CC, followed by melt-annealing for in-situ growth of agCu(MeIm)2 on the surface of the CC. Thanks to the intrinsic binding property of MOF glasses, the agCu(MeIm)2-CC containing free nonconductive binder (e.g., Nafion) exhibits an exceptionally high NH3 partial current density (jNH3) of-1207 mA cm-2 at constant current electrolysis measurements. Compared to crystalline Cu(MeIm)2, the MOF glass-derived Cu nanoparticles retain a lower coordination number (2.3 versus 6.3) after electrocatalytic reconstruction, which enhances NO3RR activity by optimizing NO3-adsorption. As a result, it achieves a high Faradaic efficiency for NH3 of 91% at-1.8 V (vs Ag/AgCl). This work represents a new exploration aimed at advancing the industrialization of the electrocatalytic reduction of NO3-to NH3 through the development of self-supporting electrodes, thereby highlighting the potential of MOF glasses in electrocatalysis.

Keyword:

ammonia copper metal-organic framework glasses nitrate electroreduction reaction self-supporting electro-des

Community:

  • [ 1 ] [Lan, Yi-Ying]Fuzhou Univ, Coll Chem, Fuzhou 350108, Fujian, Peoples R China
  • [ 2 ] [Chen, Wei-Xuan]Fuzhou Univ, Coll Chem, Fuzhou 350108, Fujian, Peoples R China
  • [ 3 ] [Si, Duan-Hui]Fuzhou Univ, Coll Chem, Fuzhou 350108, Fujian, Peoples R China
  • [ 4 ] [Huang, Yuan-Biao]Fuzhou Univ, Coll Chem, Fuzhou 350108, Fujian, Peoples R China
  • [ 5 ] [Cao, Rong]Fuzhou Univ, Coll Chem, Fuzhou 350108, Fujian, Peoples R China
  • [ 6 ] [Lan, Yi-Ying]Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China
  • [ 7 ] [Chen, Wei-Xuan]Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China
  • [ 8 ] [Si, Duan-Hui]Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China
  • [ 9 ] [Zhu, Hong-Jing]Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China
  • [ 10 ] [Fu, Xiao-Xue]Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China
  • [ 11 ] [Huang, Yuan-Biao]Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China
  • [ 12 ] [Cao, Rong]Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China
  • [ 13 ] [Si, Duan-Hui]Fujian Sci & Technol Innovat Lab Optoelect Informa, Fuzhou 350108, Fujian, Peoples R China
  • [ 14 ] [Huang, Yuan-Biao]Fujian Sci & Technol Innovat Lab Optoelect Informa, Fuzhou 350108, Fujian, Peoples R China
  • [ 15 ] [Cao, Rong]Fujian Sci & Technol Innovat Lab Optoelect Informa, Fuzhou 350108, Fujian, Peoples R China
  • [ 16 ] [Zhu, Hong-Jing]Univ Chinese Acad Sci, Beijing 100049, Peoples R China
  • [ 17 ] [Fu, Xiao-Xue]Univ Chinese Acad Sci, Beijing 100049, Peoples R China
  • [ 18 ] [Huang, Yuan-Biao]Univ Chinese Acad Sci, Beijing 100049, Peoples R China
  • [ 19 ] [Cao, Rong]Univ Chinese Acad Sci, Beijing 100049, Peoples R China

Reprint 's Address:

  • [Cao, Rong]Fuzhou Univ, Coll Chem, Fuzhou 350108, Fujian, Peoples R China;;[Cao, Rong]Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China;;[Cao, Rong]Fujian Sci & Technol Innovat Lab Optoelect Informa, Fuzhou 350108, Fujian, Peoples R China;;[Cao, Rong]Univ Chinese Acad Sci, Beijing 100049, Peoples R China

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Source :

CCS CHEMISTRY

Year: 2025

9 . 4 0 0

JCR@2023

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 2

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