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Original Experimental Approach for Assessing Transport Fuel Stability
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Efficient destruction of basic organo-nitrogenous compounds in liquid hydrocarbon fuel using ascorbic acid/H2O2
Xin Jin1, Xiaohu Du1, Guangrong Liu1
1Yunnan Key Laboratory of Carbon Neutrality and Green Low-carbon Technologies, School of Materials and Energy, Yunnan University, Kunming 650091, PR China.
Journal of Hazardous Materials
|August 10, 2023
Summary
A novel oxidative denitrogenation method effectively removes organo-nitrogenous compounds from liquid fuels using ascorbic acid and hydrogen peroxide. This ambient condition process shows high efficiency for basic compounds, offering a promising alternative to conventional refinery methods.
Area of Science:
- Green Chemistry
- Catalysis
- Environmental Science
Background:
- Conventional refinery methods for removing organo-nitrogenous compounds (ONCs) face limitations.
- Development of efficient and environmentally friendly denitrogenation techniques is crucial for liquid fuels.
Purpose of the Study:
- To introduce a novel oxidative denitrogenation (ODN) method for removing ONCs from liquid fuels.
- To evaluate the efficacy of an ascorbic acid (AscH2) and hydrogen peroxide (H2O2) redox system under ambient conditions.
- To elucidate the reaction pathway for ONC degradation.
Main Methods:
- Utilized an AscH2/H2O2 redox system for ODN of seven selected ONCs.
- Conducted experiments under ambient temperature (30°C) and atmospheric pressure.
- Employed free radical quenching and electron paramagnetic resonance (EPR) to identify active species.
- Analyzed degradation products of quinoline using GC-MS and ion chromatography.
Main Results:
- Achieved >95% removal of basic ONCs (pyridine, quinoline, acridine).
- Demonstrated moderate removal (61-68%) for water-soluble ONCs (7,8-benzoquinoline, NMP, DMF).
- Confirmed the significant role of hydroxyl and AscH2 radicals in ONC degradation.
- Proposed a three-step reaction pathway for quinoline degradation: N-onium formation, transfer hydrogenation, and oxidative ring-opening.
Conclusions:
- The AscH2/H2O2 system offers an effective, ambient condition method for ODN.
- The process shows selective removal capabilities, particularly for basic ONCs.
- This approach holds potential for pre-denitrogenation and selective removal in fuel oils.
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