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基于核酸适配体功能化荧光氧化石墨烯的免标记“Turn-off”型Hg2+传感器研究
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作者单位
杨梅,张何,雷湘玲,傅昕,王青,周宁涛 湖南工程学院化学化工学院湖南省环境催化与废弃物再生化重点实验室 
基金项目:国家自然科学基金项目(21005067);湖南省自然科学基金资助项目(2019JJ40055);湖南省教育厅资助科研项目(17A044,16B060)
中文摘要:利用湿化学法制备出具有一定荧光性能的氧化石墨烯(GO)负载金纳米颗粒(AuNPs)复合材料(GO@AuNPs),并将巯基化单链富T核酸适配体(aptamer)结合在该复合材料的金纳米颗粒表面,形成aptamer功能化氧化石墨烯-金纳米颗粒复合物(aptamer-GO@AuNPs)。当汞离子存在时,由于7个T-Hg2+-T结构的配位作用,aptamer折叠形成刚性的发夹状双链DNA结构,并使Hg2+靠近石墨烯表面(少于1 nm),使得电子可沿着双链DNA通道从石墨烯转移到汞离子,从而猝灭氧化石墨烯的荧光,由此构建了一种基于石墨烯荧光猝灭的“turn off”型荧光传感器。考察了多种因素对检测体系的影响,在最优实验条件下,此方法对Hg2+的线性检测范围为0.5~80 nmol/L,检出限为0.3 nmol/L。应用于环境水体样品中Hg2+的检测,加标回收率为96.0%~105%,相对标准偏差为1.4%~3.2%。该方法操作简单,有较强的抗干扰能力,灵敏度和选择性高,不需要标记,检测快速,可用于环境水体样品中Hg2+的高灵敏检测。
中文关键词:氧化石墨烯;核酸适配体;金纳米颗粒;免标记  Hg2+;荧光猝灭
 
Label-free Detection of Hg2+ Using a “Turn-off”Fluorescent Sensor Based on Aptamer Functionalized Graphene Oxide
Abstract:In this study,a “turn off” fluorescent sensor based on aptamer functionalized grapheme oxide(GO) decorated gold nanoparticles(AuNPs) composites was developed for the detection of Hg2+.Firstly,the GO@AuNPs with certain fluorescence properties were fabricated by wet chemical method,then the sulfhydryl modified single chain T-rich nucleic acid DNA(aptamer) was immobilized on the surface of gold nanoparticles to form aptamer functionalized graphene oxide decorated gold nanoparticles complexes(aptamer-GO@AuNPs).In the presence of Hg2+,due to the coordination of seven T-Hg2+-T structures,T-rich aptamer was folded to form a rigid and double stranded hairpin structure,making coordinated Hg2+ close to the graphene surface(less than 1 nm).In that case,electrons could transfer from graphene to mercury ion along the double stranded DNA channel,which caused the graphene fluorescence quenched.Based on this,a “turn-off” fluorescence sensor was constructed.Under the optimal experimental conditions,the linear detection range for Hg2+ was 0.5-80 nmol/L,and the detection limit was 0.3 nmol/L.The method was applied in the detection of Hg2+ in environmental water samples.The recoveries ranged from 96.0% to 105% with the relative standard deviations of 1.4%-3.2%.With the advantages of simple operation,strong anti-interference,high sensitivity and selectivity,label-free and rapid detection,the method could be used for the high sensitive detection of Hg2+ in environmental water samples.
Key Words:graphene oxide  aptamer  gold nanoparticles  label-free  Hg2+  fluorescence quenching
引用本文:杨梅,张何,雷湘玲,傅昕,王青,周宁涛.基于核酸适配体功能化荧光氧化石墨烯的免标记“Turn-off”型Hg2+传感器研究[J].分析测试学报,2019,38(10):1200-1206.
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