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Ketazine-Linked Covalent Organic Framework for Metal-Free Electrocatalytic Nitrate-to-Ammonia Conversion
Islam E Khalil1, Ashadul Adalder2, Badr Elkamash3,4
1Department of Chemistry, Functional Materials Technische Universität Berlin, Berlin, Germany.
We developed a novel, metal-free covalent organic framework (COF) for efficient electrocatalytic nitrate reduction. This sustainable material converts nitrate to ammonia, offering a greener alternative for chemical synthesis and environmental remediation.
Area of Science:
- Materials Science
- Electrochemistry
- Green Chemistry
Background:
- Electrocatalytic nitrate reduction (NO3RR) offers sustainable ammonia synthesis and nitrate remediation.
- Covalent organic frameworks (COFs) show promise for NO3RR due to tunable porosity and active sites.
- Existing COF catalysts often rely on metal active sites, limiting sustainability.
Purpose of the Study:
- To introduce a novel, metal-free COF for highly active NO3RR.
- To investigate the impact of fluorination on COF structure and catalytic performance.
- To demonstrate a sustainable alternative to metal-based electrocatalysts.
Main Methods:
- Synthesis of a fluorinated ketazine-linked COF (F-Ketazine COF) via solvothermal reaction.
- Characterization of the F-Ketazine COF's crystallinity and structural properties.
- Electrocatalytic evaluation of the F-Ketazine COF for NO3RR under neutral pH conditions.
Main Results:
- The F-Ketazine COF exhibited superior crystallinity and enhanced electrocatalytic activity compared to its non-fluorinated counterpart.
- Achieved 59.9% Faradaic efficiency for ammonia (NH3) production.
- Reached an NH3 yield rate of 1639.9 µmol h⁻¹ mgCOF⁻¹ at -0.9 V versus RHE.
Conclusions:
- This work presents the first ketazine-linked COF for electrocatalysis and the first metal-free COF for NO3RR.
- Fluorinated ketazine linkages are effective in developing sustainable and efficient COF-based electrocatalysts.
- The F-Ketazine COF demonstrates significant potential for green ammonia synthesis and nitrate remediation.
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