基于纳米孔金与离子印迹聚合物结合的新型电化学传感器用于测定砷离子(III)
收稿日期: 2019-12-21
修回日期: 2020-06-03
网络出版日期: 2020-06-04
基金资助
国家重点研发计划项目资助No(2016YFC0400704)
Novel Electrochemical Sensor Based on Integration of Nanoporous Gold with Molecularly Imprinted Polymer for Detection of Arsenic Ion(III)
Received date: 2019-12-21
Revised date: 2020-06-03
Online published: 2020-06-04
砷是一种有毒的化学元素,尤其对环境和人体健康有害. 因此,简单、快速和准确的砷离子（As3+）检测方法的开发引起了广泛的关注. 本项工作研究了基于离子印迹聚合物（MIP）和纳米多孔金（NPG）改性氧化铟锡（ITO）电极（MIP/NPG/ITO）用于检测不同水质中砷离子（As3+）测定的电化学传感器. 通过步骤简单、易操控、绿色环保的电沉积方法在ITO表面原位制备具有高导电,大比表面积,高生物相容性的NPG. 然后通过电聚合在NPG表面上原位合成一层MIP,其中As3+用作模板分子,邻苯二胺用作功能单体. 通过扫描电镜（SEM）和能谱仪（EDS）对MIP/NPG/ITO的制备过程进行了跟踪. 采用铁氰化钾与亚铁氰化钾螯合物作为电化学探针产生信号,采用循环伏安法（CV）和电化学阻抗谱（EIS）研究了MIP/NPG/ITO的电化学行为. 通过优化实验条件,采用循环伏安法对As3+进行了定量检测,其测量As3+的线性范围为2.0×10-11至9.0×10-9 mol·L-1,检测下限为7.1×10-12 mol·L-1（S/N = 3）. 所构建传感器的检出限远低于10 ppb,符合世界卫生组织（WHO）和环境保护局（EPA）设定的饮用水标准. 另外,该传感器具有制备和确定步骤简单,重复性好,重现性和稳定性优异的优点. 值得一提的是,所制备的传感器已成功应用于测量景观河水、地下水、自来水和生活污水等四种水质中As3+. 可以预见,这种简单而廉价的传感器在环境监测,食品分析和临床诊断领域具有潜在的实际应用价值.
马武威 , 常启刚 , 史雄芳 , 童延斌 , 周立 , 叶邦策 , 鲁建江 , 赵金虎 . 基于纳米孔金与离子印迹聚合物结合的新型电化学传感器用于测定砷离子(III)[J]. 电化学, 2020 , 26(6) : 900 -910 . DOI: 10.13208/j.electrochem.191221
Arsenic, a toxic chemical element, is detrimental to environment and human health in particular. Therefore, the development of simple, fast, and accurate arsenic ion (As3+) detection methods has attracted extensive attention. In this work, an electrochemical sensor based on molecular imprinted polymer (MIP) and nano-porous gold (NPG) modified indium tin oxide (ITO) electrode (MIP/NPG/ITO) was developed for determination of As3+ in water with different quality. NPG with high conductivity, large specific surface area and high biocompatibility was prepared in situ on ITO surface by a green electrodeposition method using simple and controllable steps. Then, a layer of MIP was synthesized in situ on NPG surface by electropolymerization, in which As3+ was used as a template molecule and mphenylenediamine as a functional monomer. The preparation process of MIP/NPG/ITO was monitored by scanning electron microscope (SEM) and energy-dispersive X-ray spectroscope (EDS). The potassium ferricyanide and potassium ferrocyanide chelates were used as electrochemical probes to generate signals. The electrochemical behavior of MIP/NPG/ITO was studied by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). After optimizing the experimental conditions, As3+ was quantitatively detected by cyclic voltammetry. The linear range of As3+ was measured from 2.0 ×10-11 to 9.0×10-9 mol·L-1, and the lower detection limit was 7.1×10-12 mol·L-1 (S/N = 3). The detection limit of the constructed sensor is far below 10 ppb, which meets the drinking water standards set by the World Health Organization (WHO) and Environmental Protection Agency (EPA). In addition, the sensor has the advantages of simple preparation, simple procedure of determination, good repeatability, excellent reproducibility and stability. It is worth mentioning that the prepared sensor has been successfully applied to the As3+ measurements of four water qualities, including landscape river water, groundwater, tap water and domestic sewage. It can be predicted that the reported simple and cheap sensor has potential practical applications in environmental monitoring, food analysis and clinical diagnosis.
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