自组装双酚A分子印迹电化学传感器研究
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摘要
双酚A (BPA)是一种典型的内分泌干扰物,具有三致效应和内分泌干扰性。目前在世界各地的水体中均有检出双酚A,其环境行为及风险评价目前成为环境领域的研究热点,但是由于双酚A在环境样品中的复杂性,寻找具有快速、高灵敏性和高选择性的现场检测的方法成为关键问题。
本文研究通过分子印迹技术制备特异识别水中痕量双酚A电化学传感器。以双酚A为模板分子,氨基丙基三乙氧基硅烷(APTES)为功能单体,正硅酸乙酯(TEOS)为交联剂,采用自组装方法,分别在铟锡氧化物(ITO)电极和碳纳米管离子液体修饰金电极表面合成双酚A分子印迹膜,标记为MIPs-ITO和MIPs-Au,制备高灵敏性和高选择性响应水体中双酚A的分子印迹电化学传感器。
电极的表面形态结构和电化学性质使用原子力显微镜和红外光谱分析仪进行表征。通过循环伏安法研究分子印迹传感器对双酚A的响应特性,结果表明,制备双酚A电化学传感器具有良好的灵敏度和选择性。MIPs-ITO电极对双酚A的浓度响应线性范围是0.5～50μgL-1,检测限是0.094μgL-1，双酚A结构相似物苯酚、对氨基苯酚和对硝基苯酚对电极结果影响很小。MIPs-Au电极对双酚A响应线性范围0.5～70μgL-1，检出限为0.072μg L-1，MIPs-Au电极对干扰物质对苯酚、对氨基苯酚、对硝基苯酚和对叔丁基苯酚的响应电流选择比分别为23.37,11.09,24.39和26.99,显示了该电极具有良好的选择性,达到了现场检测水中双酚A的标准。
本研究使用自组装方法制备双酚A分子印迹聚合物,使用碳纳米管和离子液体修饰电极表面,发展了一种检测水体中双酚A的新方法。本研究为水体中的双酚A的高灵敏度选择性现场检测提供重要的技术支撑,对实现准确快速的突发环境事件预警、环境风险评价具有重要意义。
Because of the mutagenic, carcinogenic, teratogenic and endocrine disrupting effects, bisphenol A (BPA) has been listed as a typical endocrine disruptor. Owing to the complexity of BPA environmental samples, highly sensitive and selective detection methods become the key issues restricted related studies.
Based on the specific recognition ability of molecularly imprinted polymers (MIPs), a novel electrochemical sensor with high sensitivity and selectivity was constructed for detection of BPA. By the approach of self-assembly, molecular imprinted polymers (MIPs) have been synthesized with BPA as template molecule,3-aminopropyltriethoxysilane (APTES) as functional monomer and tetraethoxysilane (TEOS) as cross linker. The MIPs film was fabricated onto an Indium tin oxide (ITO) electrode (MIPs-ITO). The MIPs film was also fabricated onto a gold electrode which modified with single-wall carbon nanotube and ionic liquids (MIPs-Au).
The BPA imprinted electrodes were characterized by AFM and FT-IR. The affinity and selectivity of the electrochemical sensors were characterized by cyclic voltammetry (CV). MIPs-ITO electrode was linear to the concentration of BPA in the range from 0.5 to 50μg L-1 and the detection limit was 0.094μg L-1. Furthermore, MIPs-ITO electrode showed low response to the interfering compounds. MIPs-Au electrode was linear to the concentration of BPA in the range from 0.5 to 70μg L-1 and the detection limit was 0.072μg L-1. At the same concentration, the current response of BPA at MIPs-Au electrode was 23.37,11.09,24.39 and 26.99 times that of phenol, p-aminophenol, p-nitrophenol and p-Tert-butylphenol respectively, which indicated that the MIPs-Au electrode performed excellent selectivity.
By the approach of self-assembly, MIP film has been synthesized fabricated onto electrode which modified with single-wall carbon nanotube and ionic liquids. This study will provide important technical support to rapid and highly sensitive field analysis of BPA in water, and has important significance for environmental risk assessment and early warning of environmental emergencies.
本文研究通过分子印迹技术制备特异识别水中痕量双酚A电化学传感器。以双酚A为模板分子,氨基丙基三乙氧基硅烷(APTES)为功能单体,正硅酸乙酯(TEOS)为交联剂,采用自组装方法,分别在铟锡氧化物(ITO)电极和碳纳米管离子液体修饰金电极表面合成双酚A分子印迹膜,标记为MIPs-ITO和MIPs-Au,制备高灵敏性和高选择性响应水体中双酚A的分子印迹电化学传感器。
电极的表面形态结构和电化学性质使用原子力显微镜和红外光谱分析仪进行表征。通过循环伏安法研究分子印迹传感器对双酚A的响应特性,结果表明,制备双酚A电化学传感器具有良好的灵敏度和选择性。MIPs-ITO电极对双酚A的浓度响应线性范围是0.5～50μgL-1,检测限是0.094μgL-1，双酚A结构相似物苯酚、对氨基苯酚和对硝基苯酚对电极结果影响很小。MIPs-Au电极对双酚A响应线性范围0.5～70μgL-1，检出限为0.072μg L-1，MIPs-Au电极对干扰物质对苯酚、对氨基苯酚、对硝基苯酚和对叔丁基苯酚的响应电流选择比分别为23.37,11.09,24.39和26.99,显示了该电极具有良好的选择性,达到了现场检测水中双酚A的标准。
本研究使用自组装方法制备双酚A分子印迹聚合物,使用碳纳米管和离子液体修饰电极表面,发展了一种检测水体中双酚A的新方法。本研究为水体中的双酚A的高灵敏度选择性现场检测提供重要的技术支撑,对实现准确快速的突发环境事件预警、环境风险评价具有重要意义。
Because of the mutagenic, carcinogenic, teratogenic and endocrine disrupting effects, bisphenol A (BPA) has been listed as a typical endocrine disruptor. Owing to the complexity of BPA environmental samples, highly sensitive and selective detection methods become the key issues restricted related studies.
Based on the specific recognition ability of molecularly imprinted polymers (MIPs), a novel electrochemical sensor with high sensitivity and selectivity was constructed for detection of BPA. By the approach of self-assembly, molecular imprinted polymers (MIPs) have been synthesized with BPA as template molecule,3-aminopropyltriethoxysilane (APTES) as functional monomer and tetraethoxysilane (TEOS) as cross linker. The MIPs film was fabricated onto an Indium tin oxide (ITO) electrode (MIPs-ITO). The MIPs film was also fabricated onto a gold electrode which modified with single-wall carbon nanotube and ionic liquids (MIPs-Au).
The BPA imprinted electrodes were characterized by AFM and FT-IR. The affinity and selectivity of the electrochemical sensors were characterized by cyclic voltammetry (CV). MIPs-ITO electrode was linear to the concentration of BPA in the range from 0.5 to 50μg L-1 and the detection limit was 0.094μg L-1. Furthermore, MIPs-ITO electrode showed low response to the interfering compounds. MIPs-Au electrode was linear to the concentration of BPA in the range from 0.5 to 70μg L-1 and the detection limit was 0.072μg L-1. At the same concentration, the current response of BPA at MIPs-Au electrode was 23.37,11.09,24.39 and 26.99 times that of phenol, p-aminophenol, p-nitrophenol and p-Tert-butylphenol respectively, which indicated that the MIPs-Au electrode performed excellent selectivity.
By the approach of self-assembly, MIP film has been synthesized fabricated onto electrode which modified with single-wall carbon nanotube and ionic liquids. This study will provide important technical support to rapid and highly sensitive field analysis of BPA in water, and has important significance for environmental risk assessment and early warning of environmental emergencies.
引文
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