Novel behavior of the chromatographic separation of linear and cyclic polymers

Montenegro-Burke, J. Rafael; Bennett, Jonathan C.; McLean, John A.; Hercules, David M.

doi:10.1007/s00216-015-9198-9

Cited by 8 publications

(4 citation statements)

References 16 publications

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“…This phenomenon has been observed in experimental studies from different groups. [81,82] Therefore, there is more evidence supporting that ring chains reach the CAP before the linear chains. This could be attributed to the smaller size of the ring, and hence less entropy loss when approaching a solid wall.…”

Section: Discussionmentioning

confidence: 99%

Comparison of Linear and Ring Polymers Partitioning into Pores Using Random Walks and Self‐Avoiding Walks Models

Litle,

Wang

2023

Macro Theory & Simulations

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We present Monte Carlo simulations that examine the partitioning of dilute solutions of ring or linear chains into a slit pore using two chain models, the random‐walk (RW) model and the self‐avoiding walk (SAW) model. We compared the partitioning coefficients K of the ring against the linear chains at the surface interaction that are both under the critical adsorption point (CAP), the exclusion regime, and above the CAP, the adsorptive regime. In both chain models, K for the ring remain larger than K for the linear chains at both regimes. The ring chain crosses over the point K = 1 at a weaker surface interaction than the linear chain. When extrapolated to infinite chain length, the cross‐over point for the ring and linear chain becomes the same (within statistical errors) for the RW model but remains different for the SAW model. The density profiles of the ring chain within the pore reveal the development of humps near the wall as the surface interaction crosses over the CAP. The excluded volume interaction in the SAW model additionally impacts the partitioning of chains in a solution consisting of a binary mixture of ring and linear chains and makes the K values in a binary mixture differ from the monodispersed solution.This article is protected by copyright. All rights reserved

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Section: Discussionmentioning

confidence: 99%

Comparison of Linear and Ring Polymers Partitioning into Pores Using Random Walks and Self‐Avoiding Walks Models

Litle,

Wang

2023

Macro Theory & Simulations

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“…Our simulations suggest that ring polymers as precursor molecules are promising canditates for the synthesis of globular soft nanoparticles for applications in nanomedicine and catalysis. While the synthesis and purification of monodisperse, unknotted and nonconcatenated rings without linear contaminants remains challenging, recent advances in isolation of ring polymers from linear chains of the same molecular weight [57][58][59][60][61][62] suggest that the synthesis of SCNPs from ring polymer precursors will be experimentally realizable in the near future.…”

Section: Discussionmentioning

confidence: 99%

Effects of precursor topology and synthesis under crowding conditions on the structure of single-chain polymer nanoparticles

Formanek

Moreno

2017

Soft Matter

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By means of molecular dynamics simulations we investigate the formation of single-chain nanoparticles through intramolecular cross-linking of polymer chains, in the presence of their precursors acting as purely steric crowders in concentrated solution. In the case of the linear precursors, the structure of the resulting SCNPs is weakly affected by the density at which the synthesis is performed. Crowding has significant effects if ring precursors are used: higher concentrations lead to the formation of SCNPs with more compact and spherical morphologies. Such SCNPs retain in the swollen state (high dilution) the crumpled globular conformations adopted by the ring precursors in the crowded solutions. Increasing the concentration of both the linear and ring precursors up to 30 % leads to faster formation of the respective SCNPs.

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“…Coupling ion mobility (IM) separation to MS (IM-MS) can provide valuable information regarding the three-dimensional structure of a polymer's architectural motif. IM-MS is capable of differentiating isomeric species, such as linear and cyclic polymers [4,5], and can provide detailed characterization regarding ion size and mass. A molecule's size and shape are described quantitatively by the gas-phase collision cross section (CCS) derived from IM measurements [6,7].…”

Section: Introductionmentioning

confidence: 99%

Alkali metal cation adduct effect on polybutylene adipate oligomers: Ion mobility-mass spectrometry

Crescentini

May

McLean

et al. 2019

Polymer

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Polyurethane (PU) di-block copolymers are one of the most versatile polymeric materials, comprised of hard and soft segments that contribute to PU's broad range of applications. Polybutylene adipate (PBA) is a commonly used soft segment in PU systems. Characterizing the structure of PBA polymers is essential to understanding complex heterogeneity within a PU sample. In this study, ion mobility-mass spectrometry (IM-MS) and tandem mass spectrometry (MS/MS) are used to structurally characterize a PBA standard (M n = 2250) adducted with a combination of monovalent alkali cations (Li, Na, K, Rb, and Cs). IM-MS profiles show unique trends associated with each cation-adducted PBA sample. Charge state trends: +1, +2, and +3 were extracted for cation-adducted PBA oligomers, and investigated to study gas-phase transitional folding. To quantitatively assess the gas-phase structural similarities and differences, a statistical test (ANOVA) was used to compare PBA oligomer-cation collisional cross sections (CCS). Fragmentation studies (MS/MS) identified the unique behavior of Li and Na for promoting 1,5 Hshift and 1,3 H-shift fragmentation, whereas the PBA precursor preferentially loses the larger K, Rb, and Cs cations as the ion activation energy is increased. The combination of adducted alkali cations, IM-MS, and MS/MS allow for unique structural characterization of this important PBA system.

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Novel behavior of the chromatographic separation of linear and cyclic polymers

Cited by 8 publications

References 16 publications

Comparison of Linear and Ring Polymers Partitioning into Pores Using Random Walks and Self‐Avoiding Walks Models

Comparison of Linear and Ring Polymers Partitioning into Pores Using Random Walks and Self‐Avoiding Walks Models

Effects of precursor topology and synthesis under crowding conditions on the structure of single-chain polymer nanoparticles

Alkali metal cation adduct effect on polybutylene adipate oligomers: Ion mobility-mass spectrometry

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