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Time-dependent surface polarization breaks static scaling relationship for selective acetylene hydrogenation.
Di Xu1,2, Max J Hülsey3, Chen Chen1,2
1Department of Chemical and Biomolecular Engineering, National University of Singapore, Singapore, Singapore.
Dynamic surface polarization enhances selectivity in palladium-catalyzed acetylene semi-hydrogenation. This method overcomes adsorption energy limits, boosting ethylene production without reducing conversion.
Area of Science:
- Heterogeneous catalysis
- Surface science
- Electrochemistry
Background:
- Controlling surface-adsorbate interactions is crucial for chemical processes.
- Static scaling correlations limit selectivity in catalysis.
- Dynamic surface polarization offers a new control strategy.
Purpose of the Study:
- To demonstrate dynamic surface polarization for overcoming adsorption energy limitations.
- To enhance selectivity in palladium-catalyzed acetylene semi-hydrogenation.
- To achieve high ethylene productivity.
Main Methods:
- Dynamic surface polarization under oscillating electric potentials.
- Acetylene semi-hydrogenation experiments.
- In situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS).
- X-ray absorption spectroscopy (XAS).
- Density functional theory (DFT) calculations.
Main Results:
- Dynamic polarization drastically enhances ethylene selectivity.
- High ethylene productivity achieved without sacrificing conversion.
- Time-dependent polarization modulates Pd electronic structure and adsorption energetics.
- Suppression of over-hydrogenation while maintaining semi-hydrogenation activity.
Conclusions:
- Dynamic electric surface modulation decouples adsorption-energy correlations.
- This strategy significantly improves heterogeneous catalysis.
- Applicable to other adsorption-mediated processes.
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