Abstract
The electrocatalytic nitrogen reduction reaction (NRR) driven by renewable electricity provides a green synthesis route for ammonia (NH3) production under ambient conditions but suffers from a low conversion yield and poor Faradaic efficiency (F.E.) because of strong competition from hydrogen evolution reaction (HER) and the poor solubility of N2 in aqueous systems. Herein, an in situ proton filter covalent organic framework catalyst (Ru-Tta-Dfp) is reported with inherent Ruthenium (Ru) sites where the framework controls reactant diffusion by suppressing proton supply and enhancing N2 flux, causing highly selective and efficient catalysis. The smart catalyst design results in a remarkable ammonia production yield rate of 2.03 mg h−1 mgcat−1 with an excellent F.E. of ≈52.9%. The findings are further endorsed with the help of molecular dynamics simulations and control COF systems without in situ proton filter feasibility. The results point to a paradigm shift in engineering high-performance NRR electrocatalysts for more feasible green NH3 production. © 2023 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH.
Original language | British English |
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Journal | Adv. Energy Mater. |
DOIs | |
State | Published - 2023 |
Keywords
- ammonia
- covalent organic framework
- electrocatalysis
- faradaic efficiency
- nitrogen reduction reaction
- Efficiency
- Electrocatalysis
- Electrocatalysts
- Molecular dynamics
- Nitrogen
- Reaction kinetics
- Reduction
- Ammonia production
- Covalent organic frameworks
- Electrocatalytic
- Electrochemicals
- Faradaic efficiencies
- Nitrogen reduction
- Nitrogen reduction reaction
- Reduction reaction
- Renewable electricity
- ]+ catalyst
- Ammonia