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An investigation of homogeneous electrocatalytic mechanism between ferrocene derivatives and l-cysteine/N-Acetyl-l-cysteine
Electrochimica Acta ( IF 5.5 ) Pub Date : 2020-03-29 , DOI: 10.1016/j.electacta.2020.136126
Shuang Yin , Peng Song , Hao Wang , Haoyu Ma , Zhan Wang , Yanmin Yu

The homogeneous electrocatalytic mechanism with a fast catalytic chemical reaction between a series of ferrocene derivatives and l-cysteine/N-Acetyl-l-cysteine (NAC) is systematically investigated. A comparison of different cyclic voltammetric waveforms is given to illustrate the interaction between kinetic parameter (λ) and excess factor (γ) in kinetic zone diagram via changing the scan rates and substrate/mediator ratio on both glassy carbon (GC) and boron doped diamond (BDD) working electrode experimentally. A split wave phenomenon is observed between ferroceneacetic acid (FAA) and l-cysteine. Also, the waveforms revealed that electron withdrawing groups (EWG) on the substrate hinders the kinetics of the homogeneous electron transfer while those on the mediator facilitates the same process. The homogeneous electrocatalytic order of the studied mediator is as follows: 1,1′-ferrocenedicarboxylic acid (FDA) > FAA > hydroxymethylferrocene (HMF) > 1-hydroxyethylferrocene (HEF) and the corresponding density functional theory (DFT) calculation is applied to support this statement. Furthermore, the second-order rate constant between FAA and l-cysteine is given by the support of numerical simulation (175 (mol m−3)−1 s−1). The present study would facilitate the understanding of homogeneous electrocatalytic process, especially those possessing a fast catalytic chemical step.



中文翻译:

二茂铁衍生物与L-半胱氨酸/ N-乙酰基-1-半胱氨酸之间均相电催化机理的研究

用一系列的二茂铁衍生物和之间的快速催化化学反应的均匀电机构-半胱氨酸/ N-乙酰基--半胱氨酸(NAC)的系统的研究。通过改变玻璃碳(GC)和掺硼金刚石的扫描速率和基质/介体比,对不同循环伏安波形的比较说明了动力学区图中动力学参数(λ)和过量因子(γ)之间的相互作用。 (BDD)实验电极。二茂铁乙酸(FAA)和l之间观察到分裂波现象-半胱氨酸。同样,这些波形表明,衬底上的吸电子基团(EWG)阻碍了均匀电子转移的动力学,而介体上的吸电子基团则促进了相同的过程。研究的介质的均相电催化顺序如下:1,1'-二茂铁二羧酸(FDA)> FAA>羟甲基二茂铁(HMF)> 1-羟乙基二茂铁(HEF),并应用相应的密度泛函理论(DFT)计算来支持这个说法。此外,FAA和1-半胱氨酸之间的二阶速率常数由数值模拟的支持给出(175(mol m -3-1  s -1)。本研究将有助于理解均相电催化过程,尤其是那些具有快速催化化学步骤的过程。

更新日期:2020-04-20
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