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.
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CCS CHEMISTRY
Year: 2025
9 . 4 0 0
JCR@2023
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ESI Highly Cited Papers on the List: 0 Unfold All
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30 Days PV: 2
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