Predicting Electrocatalytic Properties: Modeling Structure-Activity Relationships of Nitroxyl Radicals

被引：94

作者：

Hickey, David P. ^{[1
]}

Schiedler, David A. ^{[1
]}

Matanovic, Ivana ^{[2
,3
]}

Phuong Vy Doan ^{[1
]}

Atanassov, Plamen ^{[2
]}

Minteer, Shelley D. ^{[1
]}

Sigman, Matthew S. ^{[1
]}

机构：

[1] Univ Utah, Dept Chem, Salt Lake City, UT 84112 USA

[2] Univ New Mexico, Dept Chem & Biol Engn, Albuquerque, NM 87131 USA

[3] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2015年 / 137卷 / 51期

关键词：

MEDIATED ELECTROOXIDATION; SELECTIVE OXIDATION; OXOAMMONIUM CATION; ALCOHOLS; POTENTIALS; MECHANISM; CATALYST; TEMPO; SALTS; MOLECULES;

D O I：

10.1021/jacs.5b11252

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Stable nitroxyl radical-containing compounds, such as 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO) and its derivatives, are capable of electrocatalytically oxidizing a wide range of alcohols under mild and environmentally friendly conditions. Herein, we examine the structure function relationships that determine the catalytic activity of a diverse range of water-soluble nitroxyl radical compounds. A strong correlation is described between the difference in the electrochemical oxidation potentials of a compound and its electrocatalytic activity. Additionally, we construct a simple computational model that is able to accurately predict the electrochemical potential and catalytic activity of a wide range of nitroxyl radical derivatives.

引用

页码：16179 / 16186

页数：8

共 53 条

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