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Highly redox-active organic molecular nanomaterials: Naphthalene and phenanthrene molecular species π-stacked MWCNT modified electrodes for oxygen-interference free H2O2 sensing in neutral pH
Journal of Electroanalytical Chemistry ( IF 4.1 ) Pub Date : 2020-12-01 , DOI: 10.1016/j.jelechem.2020.114680
Sivakumar Nisha , Annamalai Senthil Kumar

Abstract Electrochemical detection of Hydrogen peroxide in neutral pH is an important analytical problem that has been often worked out using horseradish peroxide (HRP) enzyme coupled with organic redox-active molecules as a transducer, and metallic systems in the form of metal nanoparticles and complexes chemically modified electrodes. Owing to non-amenable characteristic, direct electrochemical oxidation/reduction of H2O2 by redox-active organic molecules has been rarely described in the literature. Herein, we report naphthalene (NaP) and phenanthrene (PhenE) moieties immobilized MWCNT as advanced organic nanomaterial systems for enzyme-free, selective (dissolved oxygen, cysteine, citric acid, ascorbic acid, uric acid and glucose-interference free) and direct electrocatalytic reduction and sensing of H2O2 in neutral pH. These new organic-materials have been prepared by multiwall carbon nanotube (MWCNT) surface-bound electrochemical oxidation of NaP and PhenE at ~1.2 V vs Ag/AgCl in pH 2 KCl-HCl solution. The “as prepared” organic molecular materials showed a highly symmetrical voltammetric signal in cyclic voltammetric technique (peak-to-peak separation potential, ΔEp = 10 mV at scan rate = 10 mV s−1) and proton-coupled electron-transfer in characteristic. These new materials were characterized using several physicochemical techniques such as FTIR and Raman spectroscopes, transmission electron-microscope and electrochemical characterization (using radical quenching molecular system, 2,2,6,6-tetramethylpiperidin-1-yl)oxidanyl (TEMPO)). From the collective experimental results, it has been revealed that cationic radical species like organic molecules are stabilized on the organic nanomaterial modified electrode surface (via strong π-π interaction) and showed the redox peak. Amperometric i-t responses of the modified electrodes showed a systematic variation in the H2O2 detection current signal with current linearity in a range of 25–300 μM. Calculated current sensitivities and regression coefficient values are 4.8 nA μM−1 and 0.9996 with NaP-Redox and 4.20 nA μM−1 and 0.9994 with PhenE-Redox systems, respectively.

中文翻译:

高氧化还原活性有机分子纳米材料:萘和菲分子种类 π 堆叠 MWCNT 修饰电极,用于在中性 pH 值下进行无氧干扰 H2O2 传感

摘要 在中性 pH 条件下过氧化氢的电化学检测是一个重要的分析问题,经常使用辣根过氧化物 (HRP) 酶与有机氧化还原活性分子偶联作为换能器,以及以金属纳米颗粒和化学配合物形式存在的金属系统。修饰电极。由于不可抗力的特性,文献中很少描述氧化还原活性有机分子对 H2O2 的直接电化学氧化/还原。在此,我们报告了固定化多壁碳纳米管的萘 (NaP) 和菲 (PhenE) 部分作为先进的有机纳米材料系统,用于无酶、选择性(无溶解氧、半胱氨酸、柠檬酸、抗坏血酸、尿酸和葡萄糖干扰)和直接电催化H2O2 在中性 pH 值下的还原和传感。这些新的有机材料是通过多壁碳纳米管 (MWCNT) 表面结合的 NaP 和 PhenE 在 pH 2 KCl-HCl 溶液中以~1.2 V vs Ag/AgCl 的电化学氧化制备的。“制备的”有机分子材料在循环伏安技术中显示出高度对称的伏安信号(峰峰值分离电位,扫描速率 = 10 mV s−1 时 ΔEp = 10 mV)和质子耦合电子转移特性. 这些新材料使用多种物理化学技术进行表征,例如 FTIR 和拉曼光谱、透射电子显微镜和电化学表征(使用自由基猝灭分子系统,2,2,6,6-四甲基哌啶-1-基)氧烷基(TEMPO)。从集体实验结果来看,研究表明,有机分子等阳离子自由基物种稳定在有机纳米材料修饰的电极表面(通过强 π-π 相互作用)并显示出氧化还原峰。改良电极的电流响应显示 H2O2 检测电流信号的系统变化,电流线性范围为 25-300 μM。计算的电流灵敏度和回归系数值分别为 4.8 nA μM-1 和 0.9996(使用 NaP-Redox),以及 4.20 nA μM-1 和 0.9994(使用 PhenE-Redox 系统)。
更新日期:2020-12-01
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