Kayaramkodath C. Ranjeesh (Author), Sukhjot Kaur (Author), Abdul K. Mohammed (Author), Safa Gaber (Author), Divyani Gupta (Author), Khaled Badawy (Author), Mohamed Aslam (Author), Nirpendra Singh (Author), Tina Škorjanc (Author), Matjaž Finšgar (Author)

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.

Keywords

covalent organic frameworks;ammonia;electrochemical synthesis;electrochemistry;nitrogen reduction reaction;ruthenium;

Data

Language: English
Year of publishing:
Typology: 1.01 - Original Scientific Article
Organization: UNG - University of Nova Gorica
UDC: 620.1/.2
COBISS: 176788227 Link will open in a new window
ISSN: 1614-6840
Views: 92
Downloads: 3
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Other data

Pages: str. 1-9
Volume: ǂVol. ǂ
Issue: ǂissue ǂ, [article no.] 2303068
Chronology: 2023
DOI: 10.1002/aenm.20230306
ID: 21627701