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1.
Anal Chem ; 96(11): 4446-4454, 2024 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-38451777

RESUMO

Microfluidic isotachophoresis (ITP) is a powerful technique that can significantly increase the reaction rate of homogeneous chemical reactions by cofocusing reactants in a narrow sample zone. Correspondingly, ITP has been utilized to reduce the reaction time in various bioanalytical assays. However, in conventional ITP, it is hardly possible to control the reaction rate in real time, i.e., speeding up or slowing down a reaction on demand. Here, we experimentally demonstrate a new mode of ITP that allows the spatial overlap of two ITP zones to be precisely controlled over time, which is a crucial first step toward controlling reaction rates. Two nonreactive samples are initially focused and separated by a spacer using a DC electric field. By superimposing an oscillating field component with sufficiently high amplitude on the DC field, the spatial overlap of their concentration profiles is temporarily increased due to electromigration dispersion. The time-average of this overlap can be precisely controlled by varying the frequency and amplitude of the oscillation. We suggest that this scheme can be transferred to chemical reactions between ionic species with sufficiently different electrophoretic mobilities. Tuning the parameters of the oscillatory electric field should allow direct control of the corresponding reaction rate.

2.
Anal Chem ; 95(19): 7575-7583, 2023 May 16.
Artigo em Inglês | MEDLINE | ID: mdl-37133530

RESUMO

Lowering the limit of detection in chemical or biochemical analysis is key to extending the application scope of sensing schemes. Usually, this is related to an increased instrumentation effort, which in turn precludes many commercial applications. We demonstrate that the signal-to-noise ratio of isotachophoresis-based microfluidic sensing schemes can be substantially increased merely by postprocessing of recorded signals. This becomes possible by exploiting knowledge about the physics of the underlying measurement process. The implementation of our method is based on microfluidic isotachophoresis and fluorescence detection, for which we take advantage of the physics of electrophoretic sample transport and the structure of noise in the imaging process. We demonstrate that by processing only 200 images, the detectable concentration, compared to the detection from a single image, is already lowered by 2 orders of magnitude without any additional instrumentation effort. Furthermore, we show that the signal-to-noise ratio is proportional to the square root of the number of fluorescence images, which leaves room for further lowering of the detection limit. In the future, our results could be relevant for various applications where the detection of minute sample amounts plays a role.

3.
Langmuir ; 36(30): 8894-8903, 2020 Aug 04.
Artigo em Inglês | MEDLINE | ID: mdl-32628852

RESUMO

Controlling the shape and position of moving and pinned droplets on a solid surface is an important feature often found in microfluidic applications. However, automating them, e.g., for high-throughput applications, rarely involves model-based optimal control strategies. In this work, we demonstrate the optimal control of both the shape and position of a droplet sliding on an inclined surface. This basic test case is a fundamental building block in plenty of microfluidic designs. The static contact angle between the solid surface, the surrounding gas, and the liquid droplet serves as the control variable. By using several control patches, e.g., like that performed in electrowetting, the contact angles are allowed to vary in space and time. In computer experiments, we are able to calculate mathematically optimal contact angle distributions using gradient-based optimization. The dynamics of the droplet are described by the Cahn-Hilliard-Navier-Stokes equations. We anticipate our demonstration to be the starting point for more sophisticated optimal design and control concepts.

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