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Determining Tribocorrosion Rate and Wear-Corrosion Synergy of Bulk and Thin Film Aluminum Alloys

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Long-Distance Rate Acceleration by Bulk Gold.

Alexander Schlimm¹, Roland Löw², Talina Rusch³

¹Christian Albrechts University Kiel, Institute of Inorganic Chemistry, Max-Eyth-Str. 2, 24118, Kiel, Germany.

Angewandte Chemie (International Ed. in English)

|February 23, 2019

Summary

Gold surfaces dramatically accelerate azobenzene cis-trans isomerization, up to 1300x faster than in solution. Tuning molecular-surface electronic coupling reveals spin-density dependent relaxation, suggesting intersystem crossing influences this catalytic effect.

Keywords:

azobenzene catalysis self-assembled monolayers surface spectroscopy vibrational spectroscopy

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Area of Science:

Surface science
Catalysis
Photochemistry

Background:

Azobenzenes undergo cis-trans isomerization, a process sensitive to their environment.
Surface catalysis can significantly alter reaction kinetics compared to solution-phase reactions.

Purpose of the Study:

To investigate the effect of a gold (Au(111)) surface on the cis-trans isomerization of azobenzenes.
To explore how varying electronic coupling to the gold surface influences isomerization rates.
To elucidate the mechanism behind the observed surface-catalyzed isomerization.

Main Methods:

Utilizing gold (Au(111)) surfaces for catalytic studies.
Designing molecular frameworks to systematically tune electronic coupling between azobenzenes and the gold surface.
Comparing isomerization kinetics in solution versus on the gold surface.

Main Results:

Observed rate acceleration of cis-trans isomerization on gold by up to a factor of 1300 compared to solution.
Isomerization kinetics for weakly coupled molecules resembled solution behavior.
For strongly coupled molecules, relaxation rates depended on spin-density distribution in triplet states, indicating intersystem crossing involvement.

Conclusions:

The gold surface acts as a potent catalyst for azobenzene isomerization.
Electronic coupling strength is a critical parameter controlling the catalytic efficiency.
The isomerization mechanism on the surface likely involves intersystem crossing, differing from solution-phase pathways.