Submicrometer Particles and Slip Flow in Liquid Chromatography

Rogers, B. A.; Wu, Zhen; Wei, Bingchuan; Zhang, Ximo; Cao, Xiang; Alabi, Oyeleye; Wirth, Mary J.

doi:10.1021/ac504683d

Cited by 44 publications

(27 citation statements)

References 21 publications

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“…Devices with ordered macropores have been employed for separation, reaction, and heat transfer. [38][39][40][41] Materials containing ordered mesopores have been applied in sensing, [42][43][44] drug release, [45][46][47][48][49] separation, [50][51][52][53][54][55][56] and catalysis. [57][58][59][60][61] 2D ordered structures like pillar arrays, bundles of fibers, and capillary bundles are, in general, arrangements in which one phase (solid or void) can be considered as formed by non-overlapping cylinders.…”

Section: Exemplary Structures Of Porous Materials 21 Ordered Structuresmentioning

confidence: 99%

Characterization of microscopic disorder in reconstructed porous materials and assessment of mass transport-relevant structural descriptors

2016

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The targeted optimization of the functional properties of porous materials includes the understanding of their transport properties and thus requires knowledge about the relationship between material synthesis, resulting in three-dimensional material morphology, and relevant transport properties. In this Perspective, we present our views and results on the characterization of microscopic disorder in functional porous materials, which are widely used today as fixed beds in adsorption, separation, and catalysis. This allows us to identify structural parameters that impact their mass transport properties and eventually their overall performance in technological operations. We address this complex topic at the following levels: (i) computer-generation of disordered packings allows the systematic investigation of the bed porosity (packing density) and degree of packing heterogeneity. These studies are complemented by the physical reconstruction of real packed and monolithic beds, which resolves the salient features of the packing process and monolith synthesis that are under the control of the experimentalist. (ii) Once reconstructed packed-bed and monolith morphologies are available, they are analysed by statistical methods to derive structural descriptors for their mass transport properties. Spatial tessellation schemes and chord length distributions are shown to be suitable for that purpose. They lead us to sensitive correlations of the degree of pore-environment heterogeneity and packing-scale disorder with the dynamics of (random) diffusion and (flow-field dependent) hydrodynamic dispersion, respectively. (iii) Direct or pore-scale numerical simulations are implemented on a highperformance computing platform to quantify the relevant transport properties of the materials. This complementary approach highlights the morphological descriptors of mass transport efficiency. They are validated by the simulations and in the future could direct the rational design of materials from their synthesis to targeted applications based on physical reconstruction.

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Section: Exemplary Structures Of Porous Materials 21 Ordered Structuresmentioning

confidence: 99%

Characterization of microscopic disorder in reconstructed porous materials and assessment of mass transport-relevant structural descriptors

2016

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“…The optimization of the LC gradient for the non-14.1 kDa ASVs is expected to improve the number of identifications with the current resin, but new SPLC resins as well as alternative resins (e.g., monoliths, 49,50 submicron silica particles 51,52 ) or LC strategies (e.g., IEC, HILIC, and UPLC) 53 are expected to provide enhanced separations and extend the platform to much larger, heavily modified proteins.…”

Section: Discussionmentioning

confidence: 99%

Continuous Elution Proteoform Identification of Myelin Basic Protein by Superficially Porous Reversed-Phase Liquid Chromatography and Fourier Transform Mass Spectrometry

et al. 2017

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Myelin basic protein (MBP) plays an important structural and functional role in the neuronal myelin sheath. Translated MBP exhibits extreme microheterogeneity with numerous alternative splice variants (ASVs) and post-translational modifications (PTMs) reportedly tied to central nervous system maturation, myelin stability, and the pathobiology of various de- and dys-myelinating disorders. Conventional bioanalytical tools cannot efficiently examine ASV and PTM events simultaneously, which limits understanding of the role of MBP microheterogeneity in human physiology and disease. To address this need, we report on a top-down proteomics pipeline that combines superficially porous reversed-phase liquid chromatography (SPLC), Fourier transform mass spectrometry (FTMS), data-independent acquisition (DIA) with nozzle-skimmer dissociation (NSD), and aligned data processing resources to rapidly characterize abundant MBP proteoforms within murine tissue. The three-tier proteoform identification and characterization workflow resolved four known MBP ASVs and hundreds of differentially modified states from a single 90 min SPLC-FTMS run on ~0.5 μg of material. This included 323 proteoforms for the 14.1 kDa ASV alone. We also identified two novel ASVs from an alternative transcriptional start site (ATSS) of the MBP gene as well as a never before characterized S-acylation event linking palmitic acid, oleic acid, and stearic acid at C78 of the 17.125 kDa ASV.

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“…The no-slip boundary condition is chosen to represent the condition of a highly wetting fluid, such as water, on a hydrophilic surface such as chromatographic silica. Slip flow (Neto et al, 2005; Voronov et al, 2006; Huang et al, 2008; Rogers et al, 2015), which is thought to occur on highly hydrophobic surfaces with hydrophilic solvents such as water, is not considered here but may lead to some degree of non-zero velocity at the particle surface when non-wetting solvent systems are employed. The flow simulation was initiated at zero velocity and iterated to a steady state.…”

Section: Models and Methodsmentioning

confidence: 99%

Transport properties and size exclusion effects in wide-pore superficially porous particles

Maier

Schure²

2018

Chemical Engineering Science

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The effects of hydrodynamic radius on the transport of solute molecules in packed beds of wide-pore superficially porous particles (SPP) are studied using pore-scale simulation. The free molecular diffusion rate varies with radius through the Stokes-Einstein relation. Lattice Boltzmann and Langevin methods are used to model fluid motion and the transport of an ensemble of solute molecules in the fluid, providing statistics on solute concentration, flux, molecule age and residence time, as a function of depth in the SPP. Intraparticle effective diffusion and bed dispersion coefficients are calculated and correlated with the hydrodynamic radius and accessible porosity. The relative importance of convection and diffusion are found to depend on the molecule (tracer) size through the diffusion rate, and convection effects are more significant for larger, slower-diffusing molecules. When larger molecules are utilized, the intraparticle concentration is reduced in proportion to the local particle porosity, leading to a natural definition of the accessible porosity used in size exclusion chromatography (SEC). Although the pore shape is complex, the SEC constant K can be calculated directly from simulation. Simulation demonstrates that the effective diffusion coefficient is elevated near the particle hull, which is largely open to interstitial flow, and decreases with depth into the particle. All molecules studied here have transport access to the entire particle depth, although the accessible volume at a given depth depends on their size. The first passage time into the particle is well predicted by the diffusion rate, but residence time is influenced by convection, shortening the average visit duration. These results are of interest in “perfusion” chromatography where convection is thought to increase separation efficiency for large biomolecules.

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Submicrometer Particles and Slip Flow in Liquid Chromatography

Abstract: Smaller particles have progressively led to higher efficiency in liquid chromatography, particularly for proteins, due to smaller diffusion distances. Particle diameter has recently entered the submicrometer region, with the back-pressure requirements alleviated by slip flow.

Cited by 44 publications

References 21 publications

Characterization of microscopic disorder in reconstructed porous materials and assessment of mass transport-relevant structural descriptors

Characterization of microscopic disorder in reconstructed porous materials and assessment of mass transport-relevant structural descriptors

Continuous Elution Proteoform Identification of Myelin Basic Protein by Superficially Porous Reversed-Phase Liquid Chromatography and Fourier Transform Mass Spectrometry

Transport properties and size exclusion effects in wide-pore superficially porous particles

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