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Steering Surface Reaction at Specific Sites with Self-Assembly Strategy.

Xiong Zhou¹, Fabian Bebensee², Mingmei Yang¹

¹BNLMS, College of Chemistry and Molecular Engineering, Peking University , Beijing 100871, China.

|August 16, 2017

Summary

This study reveals that specific silver surface sites exhibit varying catalytic activity. The research demonstrates control over chemical reactions by directing intermediates to more active hollow sites on the Ag(111) surface.

Keywords:

Ullmann coupling active site scanning tunneling microscopy self-assembly strategy steering surface reaction

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Area of Science:

Surface Science
Catalysis
Computational Chemistry

Background:

Understanding active site behavior is crucial for controlling surface reactions.
Self-assembly strategies can confine reactants to specific surface locations.

Purpose of the Study:

To investigate the catalytic activity of different active sites on an atomically flat silver surface.
To control chemical reactions by site-steering intermediates.

Main Methods:

Utilized a self-assembly strategy to study the Ullmann coupling of 4-bromobiphenyl.
Employed scanning tunneling microscopy (STM), synchrotron X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations.
Analyzed the catalytic cycle involving organometallic intermediates.

Main Results:

Identified that intermediates self-assemble on either 2-fold bridge or 3-fold hollow sites.
Determined that the 3-fold hollow sites are catalytically more active than the 2-fold bridge sites.
Achieved site-steered reaction control, forming p-quaterphenyl at specific temperatures.

Conclusions:

The catalytic activity of surface sites can be differentiated and controlled.
Site-specific confinement of intermediates is a viable strategy for reaction control.
This work provides insights into surface-catalyzed reactions and material design.