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Hydrogen Electrooxidation in Ionic Liquids Catalyzed by the NTf2 Radical.
Yongan Tang1, Lu Lin1, Anil Kumar1
1Department of Chemistry, Oakland University, Rochester, Michigan 48309, United States.
The Journal of Physical Chemistry. C, Nanomaterials and Interfaces
|October 27, 2017
Summary
A novel catalytic mechanism for hydrogen electrooxidation was discovered in an ionic liquid. A platinum-bound radical intermediate significantly enhances hydrogen oxidation rates, confirmed by experimental and theoretical studies.
Area of Science:
- Electrochemistry
- Catalysis
- Ionic Liquids
Background:
- Hydrogen electrooxidation is crucial for energy technologies.
- Understanding reaction mechanisms is key to improving efficiency.
- Aprotic ionic liquids offer unique electrochemical environments.
Purpose of the Study:
- To investigate the mechanism of hydrogen electrooxidation in [Bmpy][NTf2].
- To identify catalytic species involved in hydrogen oxidation.
- To elucidate the role of ionic liquid components in the reaction.
Main Methods:
- Cyclic voltammetry was used for experimental investigation.
- Density functional theory (DFT) calculations were employed for theoretical analysis.
- Electrochemical studies were conducted under anaerobic conditions.
Main Results:
- A platinum-bound NTf2 radical (NTf2•) was identified as a key intermediate.
- This radical species was found to catalyze hydrogen electrooxidation.
- The radical significantly enhanced the hydrogen oxidation reaction rate.
- Both experimental and DFT results supported the proposed radical mechanism.
Conclusions:
- The hydrogen abstraction mechanism involving a NTf2• radical is supported.
- This radical intermediate plays a crucial role in catalyzing hydrogen redox processes.
- The findings offer insights into designing efficient electrocatalysts in ionic liquids.
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