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Published on: June 12, 2019
Boosting photocatalytic nitrogen reduction reaction by Jahn-Teller effect.
Li Wang1, Ben Ma1, Yiran Teng2
1Jiangsu Collaborative Innovation Center of Atmospheric Environment and Equipment Technology (CICAEET), Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control (AEMPC), Joint International Research Laboratory of Climate and Environment Change (ILCEC), Jiangsu Engineering and Technology Research Center of Environmental Cleaning Materials (ECM), School of Environmental Science and Engineering, Nanjing University of Information Science and Technology, 219 Ningliu Road, Nanjing 210044, China.
Photocatalytic ammonia production using MoO3·0.55H2O shows enhanced nitrogen reduction reaction (NRR) rates. This sustainable method utilizes distorted crystal structures for improved N2 activation and ammonia synthesis.
Area of Science:
- Materials Science
- Catalysis
- Green Chemistry
Background:
- The Haber-Bosch process, while traditional, is energy-intensive.
- Photocatalytic ammonia production offers a sustainable alternative with lower energy demands.
- Nitrogen reduction reaction (NRR) is key to sustainable ammonia synthesis.
Purpose of the Study:
- To investigate the photocatalytic nitrogen reduction reaction (NRR) on MoO3·0.55H2O and α-MoO3.
- To understand the structure-activity relationship in photocatalytic ammonia production.
- To evaluate the efficiency of MoO3·0.55H2O as a photocatalyst for NRR.
Main Methods:
- Synthesis and structural analysis of MoO3·0.55H2O and α-MoO3.
- X-ray photoelectron spectroscopy (XPS) to identify active sites.
- Photocatalytic activity testing under visible light, including transient photocurrent, photoluminescence, and electrochemical impedance spectra (EIS).
- Density functional theory (DFT) calculations for adsorption studies.
Main Results:
- MoO3·0.55H2O exhibits distorted [MoO6] octahedrons, creating Lewis acid sites favorable for N2 adsorption.
- MoO3·0.55H2O shows higher charge separation and transfer efficiency compared to α-MoO3.
- An ammonia production rate of 88.6 μmol·gcat-1 was achieved with MoO3·0.55H2O, 4.6 times higher than α-MoO3, without sacrificial agents.
Conclusions:
- The distorted crystal structure of MoO3·0.55H2O enhances Lewis acid sites, improving N2 activation and photocatalytic NRR.
- MoO3·0.55H2O demonstrates superior photocatalytic performance for ammonia synthesis under visible light.
- This study provides insights into designing efficient photocatalysts based on crystal fine structure for sustainable ammonia production.
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