Brownian Sieving Effect for Boosting the Performance of Microcapillary Hydrodynamic Chromatography. Proof of Concept

Biagioni, Valentina; Sow, Alpha L.; Adrover, Alessandra; Cerbelli, Stefano

doi:10.1021/acs.analchem.1c00780

Cited by 10 publications

(6 citation statements)

References 37 publications

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“…A validation of the Langevin approach to model particle dynamics in confined microfluidic geometries is discussed in ref , where numerical predictions are compared to results of experiments performed in deterministic lateral displacement devices. Details of the numerical approach can be found in the Supporting Information of ref . By the Fokker-Plank theorem, the spatiotemporal dynamics of a large number of particles governed by eq yields the particle number density function, c ( x , y , z , t ), solution of the microtransport eq .…”

Section: Materials and Methodsmentioning

confidence: 99%

50-Fold Reduction of Separation Time in Open-Channel Hydrodynamic Chromatography via Lateral Vortices

Biagioni

Cerbelli

2022

Anal. Chem.

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Despite its relatively long history, open-channel hydrodynamic chromatography (OC-HDC) still represents a niche technique for determining the size distribution of particle suspensions. Practical limitations of this separation method ultimately arise from the low eluent velocity that is necessary to contain the adverse increase of analyte bandwidth caused by Taylor-Aris dispersion. Because of the micrometric size of the channel cross section, the low eluent velocity translates into order of pL-per-minute flow rates, which introduce a challenge for both the injection and the detection systems. In this article, we provide theoretical/numerical evidence illustrating how a sizable reduction of the Taylor-Aris effect can be obtained by triggering crosssectional vortices alongside the main pressure-driven axial flow. As a case study, we consider a square channel geometry where the lateral vortices are created by DC-induced electroosmosis. The analysis of particle separation is based on the classical excludedvolume macrotransport approach, which allows to derive the average particle velocity and the axial dispersion coefficient from the solution of two stationary advection-diffusion problems defined onto the channel cross section. We find that lateral vortices can enhance the separation efficiency quantitatively, e.g., by reducing the separation time of a two-species mixture by a 50-fold factor compared to standard OC-HDC.

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Section: Materials and Methodsmentioning

confidence: 99%

50-Fold Reduction of Separation Time in Open-Channel Hydrodynamic Chromatography via Lateral Vortices

Biagioni

Cerbelli

2022

Anal. Chem.

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“…The effective transport parameter

W_{p}^{eff}

and

D_{p}^{eff}

can be computed 12–15 from the velocity field w ( x , y ) and the so called b ‐field b ( x , y ).

true \begin{matrix} center W_{normalp}^{normaleff} = \frac{\int_{{normalΩ}_{normalp}} w (x, y) normald x normald y}{\int_{{normalΩ}_{normalp}} normald x normald y}, & center \begin{matrix} center D_{normalp}^{normaleff} = D_{normalp} + D_{normalp} \frac{\int_{{normalΩ}_{normalp}} {| | \nabla_{⊥} b | |}^{2}}{\int_{{normalΩ}_{normalp}} normald x normald y} \\ center = D_{normalp} + \frac{\int_{{normalΩ}_{normalp}} b (W_{p}^{eff} - w) normald x normald y}{\int_{{normalΩ}_{normalp}} normald x normald y} \end{matrix} \end{matrix}

…”

Section: Theoretical Settingmentioning

confidence: 99%

“…This initial column segment length L T ( d p ) necessary for medium ( d p = d 2 ) and small particles ( d p = d 3 ) to reach a uniform distribution on the accessible cross‐sectional domain Ω p can be estimated as 13, 14:

true \begin{matrix} center L_{normalT} (d_{p}) \approx H \frac{P e_{normalp}}{ν_{normalp}}, & center P e_{normalp} = \frac{UH}{D_{p}} \end{matrix}

…”

Section: Theoretical Settingmentioning

confidence: 99%

“…HDC is commonly applied for the characterization of polymer mixtures, however, it requires lengthy channels to obtain an adequate resolution between particles of different size. Recently, a new device with a two-coaxial channel geometry has been designed [14][15][16], where the HDC separation drive is combined with a Brownian sieving (BS) mechanism to boost the efficiency of the separation between particles below and above a critical size. Enhancement factors of order 20 with respect to the standard HDC device have been predicted, meaning that the BS-HDC column length is 2000 % shorter than the HDC capillary [14] with the same resolution (separation efficiency).…”

Section: Introductionmentioning

confidence: 99%

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Fractionation of a Three‐Particle Mixture by Brownian Sieving Hydrodynamic Chromatography

et al. 2023

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Particles ranging in size from a few nanometers (exosomes or viruses) to a few micrometers (bacteria or red blood cells) can be sorted using a size-based separation process. One of the simplest techniques is provided by hydrodynamic chromatography (HDC) which typically requires long channels to achieve adequate resolution. A new separation mechanism based on a Brownian sieving effect coupled with HDC has recently been proposed to overcome these limitations. An efficiency improvement of up to 2000 % has been predicted for a two-size mixture. The aim of this work is to study and optimize a modified geometry useful for obtaining the simultaneous separation of a three-size diluted suspension. The results suggest a significant performance improvement, up to 3000 %, over the standard HDC.

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“…[7][8][9] The miniaturization of analytical devices, reducing the device dimension, solvent consumption and analysis time, has moved the attention toward the analysis and characterization of the transient behavior of dispersion properties because asymptotic conditions are not always achieved on the length-scales of the device. [10][11][12] Moreover, when the time scales of experimental observations reduce together with the device dimensions, the accurate description of transient phenomena becomes more and more important for a correct interpretation of experimental results. 13,14 Multiple-scale expansion, 15,38 volume averaging, [16][17][18] and Brenner's moment analysis 19 are all equivalent strategies [20][21][22] for identifying the long-term properties of advecting-diffusing fields, i.e., for reducing a transport problem, in its asymptotic regime, from the indefinite propagation in R n to a cell problem in a bounded domain X 2 R n .…”

Section: Introductionmentioning

confidence: 99%

Exact moment analysis of transient/asymptotic dispersion properties in periodic media with adsorbing/desorbing walls

2022

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The paper develops a robust and computationally efficient homogenization approach, grounded on exact local and integral moments, to investigate the temporal evolution of effective dispersion properties of solute particles in periodic media possessing absorbing/desorbing walls. Adsorption onto and desorption from active walls allow linear and reversible mass transfer between the solid surface and the fluid phase. The transient analysis reveals some important features of the dispersion process that cannot be captured by asymptotic approaches aimed at determining exclusively the long-range/large-distance dispersion properties. Two case studies are considered: the dispersion of an analyte in a sinusoidal channel with adsorbing/desorbing walls and the retentive pillar array column for liquid chromatography. For both systems, the transient analysis shows how the tortuous fluid motion induced by the sinusoidal walls or by the presence of pillars induces wide and persistent temporal oscillations of the effective velocity and dispersion coefficient even for a steady (non-pulsating) Stokes flow. The adsorption/desorption process strongly amplifies the phenomenon of the overshoot for the effective dispersion coefficient that, on short/intermediate time scales, reaches values significantly larger than the asymptotic one. Moreover, the method proposed allows a detailed analysis of the temporal evolution of the skewness of the marginal distribution of the analyte along the main stream direction. It clearly shows that the time scale for achieving the macro-transport regime, which implies a Gaussian (symmetric) marginal pdf, is largely underestimated if one bases the analysis on the attainment of constant asymptotic values for the effective velocity and for the dispersion coefficient.

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Brownian Sieving Effect for Boosting the Performance of Microcapillary Hydrodynamic Chromatography. Proof of Concept

Cited by 10 publications

References 37 publications

50-Fold Reduction of Separation Time in Open-Channel Hydrodynamic Chromatography via Lateral Vortices

50-Fold Reduction of Separation Time in Open-Channel Hydrodynamic Chromatography via Lateral Vortices

Fractionation of a Three‐Particle Mixture by Brownian Sieving Hydrodynamic Chromatography

Exact moment analysis of transient/asymptotic dispersion properties in periodic media with adsorbing/desorbing walls

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