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Interfacial Lewis Acid-Base Adduct Formation Probed by Vibrational Spectroscopy
Joel G Patrow1, Yi Wang1, Jahan M Dawlaty1
1Department of Chemistry , University of Southern California , Los Angeles , California 90007 , United States.
The Journal of Physical Chemistry Letters
|June 14, 2018
Summary
Surface Lewis pair (LP) interactions are weaker than in bulk, impacting surface reactions. This study probes interfacial adducts using vibrational spectroscopy, revealing key factors influencing these weaker interactions.
Area of Science:
- Surface Chemistry
- Spectroscopy
- Materials Science
Background:
- Controlling surface reactions is crucial for many chemical processes.
- Lewis pair (LP) interactions are fundamental to chemical bonding and reactivity.
- Understanding LP interactions at interfaces is key to designing heterogeneous catalysts and surfaces.
Purpose of the Study:
- To investigate the strength of Lewis pair interactions at a heterogeneous interface.
- To compare surface LP adducts with their bulk counterparts.
- To identify factors influencing interfacial LP interactions.
Main Methods:
- Formation of interfacial Lewis adducts using tris(pentafluorophenyl)borane (Lewis acid) and 4-mercaptobenzonitrile on gold (Lewis base).
- Utilizing sum frequency generation (SFG) spectroscopy to measure vibrational frequency shifts of the nitrile group as a probe of adduct strength.
- Comparing frequency shifts of surface adducts with bulk adducts.
Main Results:
- Surface adducts exhibited a distinctly smaller vibrational frequency shift compared to bulk adducts.
- This indicates a weaker Lewis acid-base interaction at the interface.
- The study explored interfacial frustration, surface electric fields, and electronic energy level alignment as potential causes.
Conclusions:
- Lewis pair interactions are weaker at the gold-organic interface compared to the bulk.
- Interfacial frustration, surface electric fields, and energy level alignment likely contribute to the observed weaker interactions.
- Findings are relevant for controlling surface reactions in heterogeneous systems.
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