Metal-Organic Framework-Based Microfluidic Impedance Sensor Platform for Ultrasensitive Detection of Perfluorooctanesulfonate

被引:108
作者
Cheng, Yu H. [2 ]
Barpaga, Dushyant [1 ]
Soltis, Jennifer A. [3 ]
Shutthanandan, V. [1 ]
Kargupta, Roli [2 ]
Han, Kee Sung [4 ]
McGrail, B. Peter [1 ]
Motkuri, Radha Kishan [1 ]
Basuray, Sagnik [2 ]
Chatterjee, Sayandev [1 ]
机构
[1] Pacific Northwest Natl Lab, Energy & Environm Directorate, Richland, WA 99352 USA
[2] New Jersey Inst Technol, Dept Chem & Mat Engn, Newark, NJ 07102 USA
[3] Pacific Northwest Natl Lab, Natl Secur Directorate, Richland, WA 99352 USA
[4] Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99352 USA
基金
美国国家科学基金会;
关键词
metal-organic frameworks; microfluidics; impedance; petfluorooctanesulfonate; sensing; detection; DIFFUSION LIMITATIONS; ADSORPTION; SORPTION; BIOSENSORS; ACIDS; PFOA; SENSITIVITY; SUBSTANCES; CHEMISTRY; WATER;
D O I
10.1021/acsami.9b22445
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
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 (ID mu E). 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.
引用
收藏
页码:10503 / 10514
页数:12
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