基于铜基金属有机框架的液栅型石墨烯晶体管高灵敏检测葡萄糖  

Highly Sensitive Detection of Glucose Using Solution-gated Graphene Transistor Based on Copper-Metal Organic Framework

作　　者：陶甜 叶嵩 马明宇 高难 蔡志伟 刘旭 常钢[1] 何云斌[1] TAO Tian;YE Song;MA Ming-Yu;GAO Nan;CAI Zhi-Wei;LIU Xu;CHANG Gang;HE Yun-Bin(Ministry-of-Education Key Laboratory for the Green Preparation and Application of Functional Materials,Hubei Key Laboratory of Polymer Materials,School of Materials Science and Engineering,Hubei University,Wuhan 430062,China)

机构地区：[1]功能材料绿色制备与应用教育部重点实验室,高分子材料湖北省重点实验室,湖北大学材料科学与工程学院,武汉430062

出　　处：《分析化学》2021年第3期387-396,共10页Chinese Journal of Analytical Chemistry

基　　金：国家自然科学基金项目(Nos.51672074,11774082,11975093);湖北省自然科学基金项目(No.2019CFA006);武汉市应用基金前沿项目(No.201801041011287)资助。

摘　　要：将金属有机框架(Metal-organic frameworks,MOFs)材料的电催化活性和液栅型石墨烯晶体管(Solution-gated graphene transistor,SGGT)的信号放大作用结合,构建了一种新型SGGT无酶葡萄糖传感器。以均苯三甲酸(BTC)为有机配体,采用溶剂热法合成铜基MOF材料(Cu-BTC),利用Nafion膜将Cu-BTC材料固定到玻碳电极上,并作为栅极,以单层石墨烯作为晶体管沟道。此传感器的传感机理是基于葡萄糖在修饰有Cu-BTC的栅电极上发生电化学反应,引起施加于SGGT的有效栅电压的变化,从而改变了沟道载流子浓度和沟道电流。由于Cu-BTC对葡萄糖良好的电催化活性及SGGT的高灵敏度,Cu-BTC修饰的SGGT传感器对葡萄糖表现出优异的传感性能,线性范围为1 nmol/L~40 mmol/L,检出限低至1 nmol/L,优于大多数传统葡萄糖检测方法。同时,此传感器对汗液和血液中的主要成分(如尿素、乳酸、多巴胺、抗坏血酸、尿酸等)表现出较好的抗干扰性能,在长期重复实验中表现出良好的稳定性,并成功应用于人体汗液中葡萄糖的检测。Cu-BTC修饰的SGGT传感器有望应用于糖尿病治疗和临床监测中的葡萄糖无酶无创检测。A novel nonenzymatic glucose sensor based on solution-gated graphene transistor(SGGT)was constructed by combining the good electrocatalytic activity of metal organic framework(MOF)materials with the signal amplification of SGGT in sensing.With trimesic acid(BTC)as the organic ligands,copper-based MOF materials(Cu-BTC)were synthesized by solvothermal method and fixed on the glassy carbon electrode with Nafion film as the gate of the device.Monolayer graphene acted as the channel of transistor.The sensing mechanism was attributed to the change of effective gate voltage applied to SGGT induced by the electrochemical reactions of glucose at the Cu-BTC modified gate electrode,thus changing the channel carrier concentration and the channel current.Due to the good electrocatalytic activity of Cu-BTC for glucose and the high sensitivity of SGGT,the SGGT sensor modified with Cu-BTC exhibited excellent sensing performance for glucose with detection limit of as low as 1 nmol/L and linear range from 1 nmol/L to 40 mmol/L,which was superior to most of the traditional glucose detection methods.Moreover,the device exhibited a good anti-interference to the main components in sweat and blood,and showed good time stability in long-term repetitive experiments.Finally,the device was successfully applied to detection of glucose in human sweat.The SGGT sensor modified with Cu-BTC was expected to be applied to non-enzyme and non-invasive detection of glucose in the realm of diabetes treatment and monitoring.

关 键 词：金属有机框架 铜 液栅型石墨烯晶体管 葡萄糖 无酶传感 无创检测 

分 类 号：O657.1[理学—分析化学] R318[理学—化学]