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Integrated Cascade Catalysts for Electrochemical Nitrate Reduction to Ammonia
Jingwen Xu1, Hengjie Liu2, Shengbo Zhang3
1Department of Applied Chemistry, School of Chemistry and Materials Science, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China.
This study introduces a novel cascade catalyst for electrocatalytic nitrate reduction, achieving high ammonia synthesis efficiency. The integrated system optimizes active hydrogen generation and utilization for zero-carbon ammonia production.
Area of Science:
- Electrochemistry
- Catalysis
- Materials Science
Background:
- Electrocatalytic nitrate reduction (NO3-RR) is a sustainable route for ammonia (NH3) synthesis.
- Challenges include sluggish proton transfer and byproduct formation, hindering efficient NH3 production.
Purpose of the Study:
- To elucidate the principles of active hydrogen generation and utilization in NO3-RR.
- To develop an integrated cascade catalytic system for enhanced NH3 electrosynthesis.
Main Methods:
- Fabrication of a catalyst with atomically dispersed Fe sites on N-doped carbon and encapsulated Ru nanoparticles.
- Electrochemical performance testing at low potentials.
- Operando SR-FTIR spectroscopy and Density Functional Theory (DFT) calculations for mechanistic studies.
Main Results:
- Achieved an NH3 yield of 2336.43 μgNH3 h-1 mgcat-1 with 96.03% Faradaic efficiency at 0 V vs RHE.
- Demonstrated enhanced NO3- affinity and accelerated hydrogenation via Fe-Ru electron transfer.
- Revealed a sustained active hydrogen generation-consumption cycle.
Conclusions:
- The integrated cascade system effectively addresses challenges in NO3-RR for NH3 synthesis.
- Mechanistic insights into active hydrogen's role in tandem catalysis are provided.
- Offers a pathway for highly selective, energy-efficient, and durable NH3 electrosynthesis and wastewater treatment.
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