材料科学
检出限
微流控
纳米孔
纳米技术
微电极
介电谱
X射线光电子能谱
吸附剂
电化学
电极
化学工程
吸附
化学
色谱法
工程类
物理化学
有机化学
作者
Yu Cheng,Dushyant Barpaga,Jennifer A. Soltis,V. Shutthanandan,Roli Kargupta,Kee Sung Han,B. Peter McGrail,Radha Kishan Motkuri,Sagnik Basuray,Sayandev Chatterjee
标识
DOI:10.1021/acsami.9b22445
摘要
The growing global concerns to public health from human exposure to perfluorooctanesulfonate (PFOS) require rapid, sensitive, in situ detection where current, state-of-the-art techniques are yet to adequately meet sensitivity standards of the real world. This work presents, for the first time, a synergistic approach for the targeted affinity-based capture of PFOS using a porous sorbent probe that enhances detection sensitivity by embedding it on a microfluidic platform. This novel sorbent-containing platform functions as an electrochemical sensor to directly measure PFOS concentration through a proportional change in electrical current (increase in impedance). The extremely high surface area and pore volume of mesoporous metal-organic framework (MOF) Cr-MIL-101 is used as the probe for targeted PFOS capture based on the affinity of the chromium center toward both the fluorine tail groups as well as the sulfonate functionalities as demonstrated by spectroscopic (NMR and XPS) and microscopic (TEM) studies. Answering the need for an ultrasensitive PFOS detection technique, we are embedding the MOF capture probes inside a microfluidic channel, sandwiched between interdigitated microelectrodes (IDμE). The nanoporous geometry, along with interdigitated microelectrodes, increases the signal-to-noise ratio tremendously. Further, the ability of the capture probes to interact with the PFOS at the molecular level and effectively transduce that response electrochemically has allowed us achieve a significant increase in sensitivity. The PFOS detection limit of 0.5 ng/L is unprecedented for in situ analytical PFOS sensors and comparable to quantification limits achieved using state-of-the-art ex situ techniques.
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