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

详细信息    查看全文

• 作者：David P. Hickey ; David A. Schiedler ; Ivana Matanovic ; Phuong Vy Doan ; Plamen Atanassov ; Shelley D. Minteer ; Matthew S. Sigman
• 刊名：Journal of the American Chemical Society
• 出版年：2015
• 出版时间：December 30, 2015
• 年：2015
• 卷：137
• 期：51
• 页码：16179-16186
• 全文大小：553K
• ISSN：1520-5126

文摘

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.