期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 136, 期 41, 页码 14432-14437出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja5053736
关键词
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资金
- Iwatani Naoji Foundation
- Kato Foundation for the Promotion of Science
- Shimadzu Science Foundation
This article introduces a carbon electrode designed to achieve efficient enzymatic electrolysis by exploiting a hierarchical pore structure based on macropores for efficient mass transfer and mesopores for high enzyme loading. Magnesium oxide-templated mesoporous carbon (MgOC, mean pore diameter 38 nm) was used to increase the effective specific surface area for enzyme immobilization. MgOC particles were deposited on a current collector by an electrophoretic deposition method to generate micrometer-scale macropores to improve the mass transfer of glucose and electrolyte (buffer) ions. To create a glucose bioanode, the porous-carbon-modified electrode was further coated with a biocatalytic hydrogel composed of a conductive redox polymer, deglycosylated flavin adenine dinucleotide-dependent glucose dehydrogenase (d-FAD-GDH), and a cross-linker. Carbohydrate chains on the peripheral surfaces of the FAD-GDH molecules were removed by periodate oxidation before cross-linking. The current density for the oxidation of glucose was 100 mA cm2 at 25 degrees C and pH 7, with a hydrogel loading of 1.0 mg cm(2). For the same hydrogel composition and loading, the current density on the MgOC-modified electrode was more than 30 times higher than that on a flat carbon electrode. On increasing the solution temperature to 45 degrees C, the catalytic current increased to 300 mA cm(2), with a hydrogel loading of 1.6 mg cm(2). Furthermore, the stability of the hydrogel electrode was improved by using the mesoporous carbon materials; more than 95% of the initial catalytic current remained after a 220-day storage test in 4 degrees C phosphate buffer, and 80% was observed after 7 days of continuous operation at 25 degrees C.
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