scholarly journals Stepwise Assembly of Heterobimetallic Complexes: Synthesis, Structure, and Physical Properties

2021 ◽  
Author(s):  
Justin L Lee ◽  
Victoria Frances Oswald ◽  
Saborni Biswas ◽  
Ethan A Hill ◽  
Joseph W Ziller ◽  
...  
Keyword(s):  
Physical Properties ◽  
Structure Function ◽  
Active Sites ◽  
Heterobimetallic Complexes ◽  
Structure Function Relationship ◽  
Function Relationship ◽  
Stepwise Assembly ◽  
Synthetic Models

Bimetallic active sites are ubiquitous in metalloenzymes and has sparked investigations of synthetic models to aid in the establishment of structure-function relationship. We previously reported a series of discrete bimetallic...

scholarly journals Substrate strain tunes operando geometric distortion and oxygen reduction activity of CuN2C2 single-atom sites

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Guokang Han ◽  
Xue Zhang ◽  
Wei Liu ◽  
Qinghua Zhang ◽  
Zhiqiang Wang ◽  
...  
Keyword(s):  
Structure Function ◽  
Oxygen Reduction ◽  
Active Sites ◽  
Geometric Distortion ◽  
Single Atom ◽  
Reduction Activity ◽  
Activity Promotion ◽  
Structure Function Relationship ◽  
Substrate Strain ◽  
Function Relationship

AbstractSingle-atom catalysts are becoming increasingly significant to numerous energy conversion reactions. However, their rational design and construction remain quite challenging due to the poorly understood structure–function relationship. Here we demonstrate the dynamic behavior of CuN2C2 site during operando oxygen reduction reaction, revealing a substrate-strain tuned geometry distortion of active sites and its correlation with the activity. Our best CuN2C2 site, on carbon nanotube with 8 nm diameter, delivers a sixfold activity promotion relative to graphene. Density functional theory and X-ray absorption spectroscopy reveal that reasonable substrate strain allows the optimized distortion, where Cu bonds strongly with the oxygen species while maintaining intimate coordination with C/N atoms. The optimized distortion facilitates the electron transfer from Cu to the adsorbed O, greatly boosting the oxygen reduction activity. This work uncovers the structure–function relationship of single-atom catalysts in terms of carbon substrate, and provides guidance to their future design and activity promotion.

Seeking a Structure-Function Relationship for γ-Al2O3 Surfaces

2018 ◽  
Author(s):  
Muhammed Acikgoz ◽  
Jaren Harrell ◽  
Michele Pavanello
Keyword(s):  
Structure Function ◽  
Active Sites ◽  
Chemical Reactivity ◽  
Surface Oxidation ◽  
Morphological Variations ◽  
Structure Function Relationship ◽  
Interesting Correlation ◽  
Surface Dipole ◽  
New Perspective ◽  
Function Relationship

<p>The subject of this work is gamma alumina surfaces. We show that surface morphological variations can induce significant changes in work function and surface dipole particularly in regards of the surface oxidation level.</p> <p>Our results offer a new perspective on the structure-function relationship between surface morphology and electronic properties. For example, and for the first time in the literature, we uncover an interesting correlation between surface dipole and chemical reactivity of the surface active sites.</p>

Seeking a Structure-Function Relationship for γ-Al2O3 Surfaces

2018 ◽  
Author(s):  
Muhammed Acikgoz ◽  
Jaren Harrell ◽  
Michele Pavanello
Keyword(s):  
Structure Function ◽  
Active Sites ◽  
Chemical Reactivity ◽  
Surface Oxidation ◽  
Morphological Variations ◽  
Structure Function Relationship ◽  
Interesting Correlation ◽  
Surface Dipole ◽  
New Perspective ◽  
Function Relationship

<p>The subject of this work is gamma alumina surfaces. We show that surface morphological variations can induce significant changes in work function and surface dipole particularly in regards of the surface oxidation level.</p> <p>Our results offer a new perspective on the structure-function relationship between surface morphology and electronic properties. For example, and for the first time in the literature, we uncover an interesting correlation between surface dipole and chemical reactivity of the surface active sites.</p>

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