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Pulsed Laser-Twisted Spinel-to-Rocksalt High-Entropy 3d-Metal Oxides for Selective Ammonia Electrosynthesis
Akash Prabhu Sundar Rajan1, Jayaraman Theerthagiri1, Wanwisa Limphirat2
1Department of Chemistry (BK21 FOUR), Research Institute of Advanced Chemistry, Gyeongsang National University, Jinju, 52828, Republic of Korea.
Small (Weinheim an Der Bergstrasse, Germany)
|June 6, 2025
Summary
Researchers developed a high-entropy rock-salt oxide (HE-RSO) catalyst for efficient electrochemical ammonia synthesis from nitrate. This novel material also enables energy generation and wastewater treatment, offering a sustainable alternative to traditional methods.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- The Haber-Bosch process is energy-intensive.
- Electrochemical nitrate reduction (eNO3RR) offers ambient ammonia synthesis.
- Nitrate-based cells can treat wastewater and generate energy.
Purpose of the Study:
- To synthesize a novel high-entropy rock-salt oxide (HE-RSO) catalyst.
- To investigate its performance in electrochemical ammonia synthesis.
- To explore its application in integrated energy systems.
Main Methods:
- Pulsed laser irradiation in liquids to create HE-RSO from 3d transition metals.
- Electrochemical testing for eNO3RR performance (ammonia production rate, Faradaic efficiency).
- In situ Raman spectroscopy and density functional theory (DFT) calculations to elucidate the catalytic mechanism.
Main Results:
- Achieved an NH3 production rate of 15.34 mg h-1 cm-2 at -0.4 V with 92% Faradaic efficiency.
- Identified Co and Cu as dual-active sites facilitating the N-end mechanism.
- Integrated the HE-RSO catalyst into a Zn-nitrate battery, yielding 1.22 V and 1.75 mW cm-2 power density.
Conclusions:
- Pulsed laser processing is effective for high-entropy material stabilization.
- HE-RSO demonstrates significant potential for sustainable ammonia production.
- The catalyst enables multifunctional applications in wastewater treatment and energy generation.
