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Plasmon-Enhanced C-C Bond Cleavage toward Efficient Ethanol Electrooxidation.
Yan Wei1, Zijie Mao1, Xian-Yin Ma1
1Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Collaborative Innovation Center of Chemistry for Energy Materials, Department of Chemistry, Fudan University, Shanghai 200438, China.
The Journal of Physical Chemistry Letters
|November 30, 2022
Summary
Localized surface plasmon resonance (LSPR) enhances electrocatalytic ethanol oxidation using visible light. Gold-platinum nanoparticles boost reaction rates and selectivity for complete ethanol oxidation under ambient conditions.
Area of Science:
- Electrochemistry
- Materials Science
- Nanotechnology
- Renewable Energy
Background:
- Ethanol is a sustainable biofuel with high energy density and environmental benefits.
- Ethanol electrooxidation suffers from slow reaction kinetics and low selectivity for complete oxidation (C1 pathway).
- Controlling reaction pathways is crucial for efficient energy conversion.
Purpose of the Study:
- To investigate the use of localized surface plasmon resonance (LSPR) to enhance ethanol electrooxidation.
- To improve reaction kinetics and selectivity towards the C1 pathway under visible light.
- To understand the molecular mechanisms of LSPR-promoted ethanol oxidation.
Main Methods:
- Utilized gold-platinum (Au@Pt) core-shell nanoparticles with a plasmonic core and active shell.
- Performed electrocatalytic ethanol oxidation in alkaline media under visible light illumination.
- Employed in situ attenuated total reflection-surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) for mechanistic studies.
Main Results:
- Illumination significantly boosted electrocatalytic activity, increasing current density from 2.30 to 4.05 A mgPt-1 at 0.8 V vs RHE.
- Visible light irradiation enhanced C1 selectivity from 9% to 38% at 0.8 V.
- In situ ATR-SEIRAS revealed LSPR's role in promoting C-C bond cleavage and subsequent CO oxidation.
Conclusions:
- LSPR effect is a viable strategy to enhance electrocatalytic ethanol oxidation kinetics and selectivity.
- Visible light activation of Au@Pt nanoparticles offers a promising route for efficient ethanol electrooxidation.
- The combination of plasmonic electrocatalysis and in situ spectroscopy provides molecular insights into reaction pathway tuning.
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