传感器类型
场效应晶体管(FET)生物传感器
检测对象
2,4-二氯苯氧乙酸(2,4-D, 2,4-dichlorophenoxyacetic acid);样品基质:PB缓冲液、土壤提取液
检测原理
SWCNT沟道电导对周围静电势高度敏感。2,4-D-BSA通过DCC/NHS共价固定于SWCNT表面,Tween-20封闭非特异位点。竞争免疫分析中,固定浓度anti-(2,4-D)抗体先与样品中游离2,4-D孵育,再注入微流控通道;游离2,4-D与固定2,4-D-BSA竞争结合抗体,游离2,4-D浓度越高,结合到SWCNT表面的抗体越少。抗体结合引入正电荷,改变SWCNT周围静电势,产生静电门控效应,使IDS-VG曲线向负栅压方向移动;在固定VG下表现为IDS下降。因此信号与免疫复合物量正相关、与游离2,4-D浓度负相关。土壤提取液离子强度差异会改变电荷屏蔽,使信号略大。
检测灵敏度
LOD: 500 fM (0.5 part-per-trillion)(2,4-D,土壤提取液);LOD: 50 pM (50 part-per-trillion)(2,4-D,PB缓冲液);LOD: 50 pM (50 part-per-trillion)(anti-(2,4-D),PB缓冲液);灵敏度斜率: 0.94% decade−1(土壤提取液);灵敏度斜率: 0.33% decade−1(PB缓冲液,2,4-D);灵敏度斜率: 0.21% decade−1(PB缓冲液,anti-(2,4-D));R^2 = 0.989(土壤提取液);R^2 = 0.995(PB缓冲液,2,4-D);R^2 = 0.957(PB缓冲液,anti-(2,4-D))
效应效果
器件选择性良好:暴露500 mM非配对牛血清白蛋白(BSA)时IDS仅轻微下降,说明Tween-20封闭有效。所有动力学测量均进行三次重复,以评估重现性;空白PB缓冲液中的漂移可离线扣除。实际土壤提取液(pH约7,电导率12 mS cm−1)中竞争免疫检测2,4-D的LOD为500 fM,缓冲液中为50 pM,均远低于WHO饮用水2,4-D最大残留限值500 nM。作者认为该全塑料LGFET结构简单、成本低,可现场部署,适用于环境样品原位分析、水中毒素检测及部分免疫诊断应用。
传感器的构成
- 基底/微流控通道:PDMS(Sylgard 134)模压微流控通道与无特征平板层压,形成柔性全塑料器件。
- 换能器电极/沟道:单壁碳纳米管(SWCNT)薄膜经SDDBS水分散液过滤成膜并转印至PDMS,形成源极、漏极和晶体管沟道。
- 电接触:注射器针尖金属段与银漆,提供源漏电极稳定电接触。
- 识别/捕获元件:2,4-D-BSA偶联物(2,4-D经DCC/NHS与BSA偶联)共价固定于SWCNT表面,作为探针捕获anti-(2,4-D)抗体。
- 识别/竞争元件:anti-(2,4-D)兔IgG抗体,与固定2,4-D-BSA结合形成免疫复合物;游离2,4-D与其竞争结合。
- 封闭剂:Tween-20封闭未结合SWCNT表面,减少非特异蛋白吸附。
- 门极/读出电极:Ag/AgCl参比电极作为液体门极施加VG,源漏偏置VDS=10 mV并测量IDS。
中文摘要
本文报道了一种用于检测2,4-二氯苯氧乙酸(2,4-D)除草剂的全塑料微流控生物传感器。器件以聚二甲基硅氧烷(PDMS)为基底和微流控通道,以层压单壁碳纳米管(SWCNT)薄膜作为源漏电极和晶体管沟道,构成液体门场效应晶体管(LGFET)。2,4-D-BSA偶联物通过DCC/NHS化学共价固定于SWCNT表面,并用Tween-20封闭非特异位点。在竞争性免疫分析中,固定浓度的anti-(2,4-D)抗体先与样品中的游离2,4-D孵育,再注入通道;游离2,4-D与固定2,4-D-BSA竞争结合抗体,免疫复合物形成引起SWCNT周围静电势变化,通过静电门控调制沟道电导,使IDS-VG曲线负移或在固定栅压下IDS下降。该传感器可实时、无标记检测液相中的2,4-D,在土壤提取液中检出限达500 fM,在缓冲液中为50 pM,显著低于WHO饮用水500 nM限值。
英文摘要
Monitoring of environmental pollutants has become increasingly important due to concern over potential health and environmental impact inflicted by these chemicals. In this contribution, we focus on the development of an all-plastic biosensor comprising laminated single-walled carbon nanotubes as the active element and its conductance modulation in a liquid-gated field effect transistor, as the principle of transduction, for the detection of 2,4-dicholorophenoxy acetic acid (2,4-D) herbicide. The reported biosensor is capable of performing real-time label-free detection of analytes in liquid environment. This biosensor which relies on immunoassay principle for specificity is able to detect down to 500 fM levels of 2,4-D in soil samples.