Investigations of electrochemical oxygen transfer reaction on boron-doped diamond electrodes
Investigations of electrochemical oxygen transfer reaction on boron-doped diamond electrodes
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DOI：
10.1016/j.electacta.2007.08.066
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发表时间：
2007-12-31
影响因子：
6.6
通讯作者：
Comninellis, Christos
中科院分区：
文献类型：
--
作者：
Kapalka, Agnieszka;Foti, Gyoergy;Comninellis, Christos
本文研究了在硼掺杂金刚石电极上，用简单碳、有机化合物（甲醇和甲酸）进行电化学氧转移反应（EOTR）。采用掺硼金刚石微电极阵列（BDD MEA）研究了析氧（副反应）和有机物氧化（主反应）的动力学。在高电位区，氧析出以120 mV dec（-1）的塔菲尔斜率和相对于H+的零反应级发生。在有机物存在下，观察到极化曲线向较低电位移动，而Tafel斜率保持接近120 mV dec（-1）。提出了一个简化的C_2有机物氧化模型。水的排放和有机物的氧化被认为是快速反应。所研究的EOTR的最慢的步骤是羟基自由基对氧的阳极放电。在本工作中，进一步介绍了甲酸在掺硼金刚石大电极上的电解。为了实现100%的电流效率，在程序电流下进行电解，其中电流密度被调节到极限值。(c)2007爱思唯尔有限公司保留所有权利。
In this paper, the electrochemical oxygen transfer reaction (EOTR) is studied on boron-doped diamond electrodes using simple C, organic compounds (methanol and formic acid). The kinetics of both oxygen evolution (side reaction) and organics oxidation (main reaction) has been investigated using boron-doped diamond microelectrodes-array (BDD MEA). Oxygen evolution, in the high-potential region, takes place with a Tafel slope of 120 mV dec(-1) and zero reaction order with respect to H+. In the presence of organics, a shift of the polarization curves to lower potentials is observed while the Tafel slopes remain close to 120 mV dec(-1). A simplified model of C, organics oxidation is proposed. Both water discharge and organics oxidation are assumed to be fast reactions. The slowest step of the studied EOTR is the anodic discharge of hydroxyl radicals to oxygen. Further in this work, electrolysis of formic acid on boron-doped diamond macroelectrode is presented. In order to achieve 100% current efficiency, electrolysis was carried out under programmed current, in which the current density was adjusted to the limiting value. (c) 2007 Elsevier Ltd. All rights reserved.