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journal article·2024-02Open access

An In situ Proton Filter Covalent Organic Framework Catalyst for Highly Efficient Aqueous Electrochemical Ammonia Production

Kayaramkodath C. Ranjeesh, Sukhjot Kaur, Abdul K. Mohammed, Safa Gaber, Divyani Gupta, Khaled Badawy, Mohamed Aslam, Nirpendra Singh, Tina Skorjanc, Matjaž Finšgar, Jésus Raya, Tharamani C. Nagaiah, Dinesh Shetty

Advanced Energy Materials· Volume 14· Issue 5
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Source abstract

Abstract

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.
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Research context

Catalysis & surfaces

OpenAlex topics: Ammonia Synthesis and Nitrogen Reduction · Advanced Photocatalysis Techniques · Covalent Organic Framework Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemistry Khalifa University Science and Technology Abu Dhabi 127788 UAE

Department of Chemistry Indian Institute of Technology Ropar Rupnagar Punjab 140001 India

Mechanical Engineering Department Khalifa University of Science and Technology Abu Dhabi 127788 UAE

Department of Physics Khalifa University of Science and Technology Abu Dhabi 127788 UAE

Materials Research Laboratory University of Nova Gorica Vipavska cesta 11c, Ajdovscina Nova Gorica 5270 Slovenia

Faculty of Chemistry and Chemical Engineering University of Maribor Smetanova ulica 17 Maribor 2000 Slovenia

Membrane Biophysics and NMR Institute of Chemistry University of Strasbourg‐CNRS Rue Blaise Pascal 1 Strasbourg cedex 67081 France

Advanced Materials Chemistry Center (AMCC) Khalifa University Science and Technology Abu Dhabi 127788 UAE

Funding

Science and Engineering Research Board · Council of Scientific and Industrial Research, India · Javna Agencija za Raziskovalno Dejavnost RS · Khalifa University of Science, Technology and Research

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