利用电化学方法开发用于灵敏检测铜(II)的特戊酸共轭 Nafion 修饰玻璃碳电极

IF 2.7 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Inorganica Chimica Acta Pub Date : 2024-08-11 DOI:10.1016/j.ica.2024.122309
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引用次数: 0

摘要

本研究利用特戊酸(pivH)分子对水介质中的铜阳离子进行电化学检测。为了实现灵敏且有选择性的电位传感器应用,在玻璃碳电极(GCE)上用导电粘合剂 nafion 制作了 pivH,使其成为对特定重金属阳离子有选择性的有效电化学探针(pivH/Nafion/GCE)。这种新制造的 pivH/Nafion/GCE 在 pH=7 的磷酸盐缓冲溶液(PBS)中,在有其他重金属阳离子干扰的情况下,对铜离子具有更强的电化学活性。在 Cu2+ 浓度从 0.1 nM 到 0.01 M 的宽线性动态范围 (LDR) 内,校准图呈线性(r2 = 0.9879);灵敏度和检测限分别为 0.0212 × 10-2 µAµM-1cm-2 和 0.014 nM。因此,这种新制作的 GCE 作为选择性电化学探针,首次利用新型电化学电流-电位(I-V)方法灵敏且选择性地检测了真实环境样品中的 Cu2+ 阳离子。此外,我们还利用特戊酸制备了新的双核铜配合物 [Cu2(piv)4(pivH)2](其中 piv = 特戊酸;pivH = 特戊酸),并通过傅立叶变换红外光谱(FTIR)、元素分析和单晶 X 射线衍射仪对其进行了表征。为了证实这些相互作用,我们进行了密度泛函理论(DFT)计算,这些计算结果与实验数据完全吻合。在 pivH 的去质子化形式中,分子静电位(MEP)分析显示静电位等于 -148.4 kcal/mol,这表明 -COOH 与铜中心有很强的相互作用。同样,相互作用能、分子中原子量子理论(QTAIM)研究和天然键轨道(NBO)分析也与实验结果一致。因此,这项新颖的研究展示了一种极佳的方法,即利用基于新设计的 pivH/Nafion/GCE 作为选择性 Cu2+ 阳离子电化学传感器的 I-V 方法,在短响应时间内对 Cu2+ 阳离子进行高选择性、高灵敏度的检测,且检测限低、重现性好。实验数据与理论计算结果吻合。
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Development of pivalic acid conjugated Nafion modified glassy carbon electrode for sensitive detection of Cu(II) by electrochemical approach

In this work, pivalic acid (pivH) molecule is employed for an electrochemical sensing of copper cations in an aqueous medium. For sensitive as well as selective potential sensor application, pivH was fabricated onto a glassy carbon electrode (GCE) facilitated by adhesive conducting binder, nafion, so as make it selective and effective electrochemical probe (pivH/Nafion/GCE) towards specific heavy metal cations. This newly fabricated pivH/Nafion/GCE reveals enhance electrochemical activity toward copper ions in the presence of other interfering heavy metal cations in phosphate buffer solution (PBS) of pH=7. The calibration plot was linear (r2 = 0.9879) across broad linear dynamic range (LDR) spanning Cu2+ concentration from 0.1 nM to 0.01 M. The sensitivity and detection limit was found to be 0.0212 × 10−2 µAµM−1cm−2 and 0.014 nM, respectively. So, this newly fabricated GCE as selective electrochemical probe offers a sensitive as well as selective detection of Cu2+ cations in real environmental samples using a novel electrochemical, current–potential (I-V), approach, for the first time. Further, we explored pivalic acid for the preparation of new di-nuclear copper complex, [Cu2(piv)4(pivH)2] (where piv = pivalate; pivH=pivalic acid) and characterized by Fourier transform infrared spectroscopy (FTIR) spectroscopy, elemental analysis and single crystal X-ray diffractometry. Density functional theory (DFT) calculations were carried out to confirm the interactions and these calculations well-support to experimental data. In case of deprotonated form of pivH, Molecular Electrostatic Potential (MEP) analysis exhibits electrostatic potential equals to −148.4 kcal/mol which suggest about the strong interaction of –COOH with copper centers. Similarly, interaction energies, the quantum theory of atoms in molecules (QTAIM) study and Natural Bond Orbital (NBO) analysis also favor to experimental work. Thus, this novel study demonstrates an excellent approach for highly selective and sensitive detection of Cu2+ cations in short response time with low detection limit and good reproducibility by using I-V method based on newly designed pivH/Nafion/GCE as selective Cu2+ cationic electrochemical sensor. The experimental data was compactable with theoretical calculations.

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来源期刊
Inorganica Chimica Acta
Inorganica Chimica Acta 化学-无机化学与核化学
CiteScore
6.00
自引率
3.60%
发文量
440
审稿时长
35 days
期刊介绍: Inorganica Chimica Acta is an established international forum for all aspects of advanced Inorganic Chemistry. Original papers of high scientific level and interest are published in the form of Articles and Reviews. Topics covered include: • chemistry of the main group elements and the d- and f-block metals, including the synthesis, characterization and reactivity of coordination, organometallic, biomimetic, supramolecular coordination compounds, including associated computational studies; • synthesis, physico-chemical properties, applications of molecule-based nano-scaled clusters and nanomaterials designed using the principles of coordination chemistry, as well as coordination polymers (CPs), metal-organic frameworks (MOFs), metal-organic polyhedra (MPOs); • reaction mechanisms and physico-chemical investigations computational studies of metalloenzymes and their models; • applications of inorganic compounds, metallodrugs and molecule-based materials. Papers composed primarily of structural reports will typically not be considered for publication.
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