Electric induced dipoles of nanocolloids the size of the Debye length are shown to be one order stronger than predicted by the classical Maxwell-Wagner theory and its extensions. The difference is attributed to normal ion migration within the diffuse layer, and adsorption onto the Stern layer at the poles. The characteristic relaxation frequency (the crossover frequency for dielectrophoresis) is shown to be inversely proportional to the RC time of the diffuse layer capacitance and resistance, and has an anomalous -1 scaling with respect to the product of the Debye length and the particle size.
Other than concentrating the target molecules at the sensor location, we demonstrate two distinct new advantages of an open-flow impedance-sensing platform for DNA hybridization on carbon nanotube (CNT) surface in the presence of a high-frequency AC electric field. The shear-enhanced DNA and ion transport rate to the CNT surface decouples the parasitic double-layer AC impedance signal from the charge-transfer signal due to DNA hybridization. The flow field at high AC frequency also amplifies the charge-transfer rate across the hybridized CNT and provides shear-enhanced discrimination between DNA from targeted species and a closely related congeneric species with three nucleotide mismatches out of 26 bases in a targeted attachment region. This allows sensitive detection of hybridization events in less than 20 min with picomolar target DNA concentrations in a label-free CNT-based microfluidic detection platform.
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.
Exploiting the functionalization chemistry of graphene, long-range electrostatic and short-range covalent interactions were harnessed to produce multifunctional energetic materials through hierarchical self-assembly of nanoscale oxidizer and fuel into highly reactive macrostructures. Specifically, we report a methodology for directing the self-assembly of Al and Bi2O3 nanoparticles on functionalized graphene sheets (FGS) leading to the formation of nanocomposite structures in a colloidal suspension phase that ultimately condense into ultradense macrostructures. The mechanisms driving self-assembly were studied using a host of characterization techniques including zeta potential measurements, X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), particle size analysis, micro-Raman spectroscopy, and electron microscopy. A remarkable enhancement in energy release from 739 ± 18 to 1421 ± 12 J/g was experimentally measured for the FGS self-assembled nanocomposites.
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