TEMPO-Modified Linear Poly(ethylenimine) for Immobilization-Enhanced Electrocatalytic Oxidation of Alcohols

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• 作者：David P. Hickey ; Ross D. Milton ; Dayi Chen ; Matthew S. Sigman ; Shelley D. Minteer
• 刊名：ACS Catalysis
• 出版年：2015
• 出版时间：September 4, 2015
• 年：2015
• 卷：5
• 期：9
• 页码：5519-5524
• 全文大小：368K
• ISSN：2155-5435

文摘

We demonstrate a method to simultaneously immobilize the oxidation catalyst, TEMPO, while dramatically enhancing its electrocatalytic activity toward several biologically available alcohols. TEMPO is covalently immobilized onto linear poly(ethylenimine), which is then cross-linked onto the surface of a glassy carbon electrode to form a hydrogel through which substrates can readily diffuse. The TEMPO-LPEI electrode is used as an anode capable of generating currents from 0.41 卤 0.06 mA cm^鈥? in the presence of 250 mM sucrose to 8.20 卤 0.04 mA cm^鈥? in the presence of 2 M methanol and 33.4 卤 9.4 mA cm^鈥? in the presence of 500 mM formate under neutral pH and at 25 掳C. The newly described anode is combined with an enzymatic biocathode to construct a hybrid biofuel cell to produce 0.38 卤 0.04 mA cm^鈥? while using 2 M methanol as a fuel source.