Gas‐phase structure of polymer ions: Tying together theoretical approaches and ion mobility spectrometry

Duez, Quentin; Hoyas, Sébastien; Josse, Thomas; Cornil, Jérôme; Gerbaux, Pascal; Winter, Julien De

doi:10.1002/mas.21745

Cited by 7 publications

(4 citation statements)

References 170 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…progress in MS, as a highly and sensitive detector, is also required. Current MS often equips a functionality of ion mobility spectrometry (IMS), a type of electrophoretic separation in the gaseous phase, and IMS-MS have been applied to various research field [62][63][64][65][66][67][68][69][70][71]. A combination of HPLC with IMS-MS(/MS) is also significant as a kind of multi-dimensional separation.…”

Section: Discussionmentioning

confidence: 99%

Development of Novel Analytical Methods Based on Liquid Chromatography and Electrophoresis

Kitagawa

2023

Chromatography

View full text Add to dashboard Cite

High-performance liquid chromatography (HPLC) and electrophoresis are liquid phase separation methods and are frequently used in various research fields. Although their origins are sufficiently old, the development of novel separation methods based on HPLC and electrophoresis are still required for both fundamental and applicational functions. In this paper, we introduced our fundamental studies of the development of novel analytical methods based on HPLC and electrophoresis toward enhancing separation efficiency. The contents can be categorized as follows: (1) enhancement of separation in pressured flow-driven capillary electrochromatography, (2) orthogonal electrochromatography for simultaneous two-dimensional separation, (3) development of new stationary phases/columns in HPLC, (4) development of low and ultra-low-temperature HPLC using liquefied gas mobile phase, (5) development of nonaqueous capillary electrophoresis for analyzing water-insoluble synthetic polymers, and (6) development of frequency division multiplex HPLC-MS.

show abstract

Section: Discussionmentioning

confidence: 99%

Development of Novel Analytical Methods Based on Liquid Chromatography and Electrophoresis

Kitagawa

2023

Chromatography

View full text Add to dashboard Cite

show abstract

“…In addition to these experimental results, molecular modeling is often used to determine the theoretical Ω value of each potential architecture. Comparison of the theoretical and experimental Ω values allows for a confident structural assignment of polymer architecture, protein folding, and molecular packing arrangement [ 33 , 34 , 35 , 36 ].…”

Section: Introductionmentioning

confidence: 99%

Elucidation of Dithiol-yne Comb Polymer Architectures by Tandem Mass Spectrometry and Ion Mobility Techniques

Williams-Pavlantos,

Mokarizadeh,

Curole

et al. 2024

Polymers

View full text Add to dashboard Cite

Polymers have a wide range of applications depending on their composition, size, and architecture. Varying any of these three characteristics can greatly impact the resulting chemical, physical, and mechanical properties. While many techniques are available to determine polymer composition and size, determining the exact polymer architecture is more challenging. Herein, tandem mass spectrometry (MS/MS) and ion mobility mass spectrometry (IM-MS) methods are utilized to derive crucial architectural information about dithiol-yne comb polymers. Based on their unique fragmentation products and IM drift times, dithiol-yne oligomers with distinct architectures were successfully differentiated and characterized. Additionally, experimental collision cross-sections (Ω) derived via IM-MS were compared to theoretically extracted Ω values from molecular dynamics simulated structures to deduce the architectural motif of these comb oligomers. Overall, this work demonstrates the benefits of combining various mass spectrometry techniques in order to gain a complete understanding of a complex polymer mixture.

show abstract

“…In particular, ion mobility spectrometry (IMS) experiments represent an invaluable analytical method to generate structural data on gas-phase ions . By comparing the measured collision cross sections (CCS) with theoretical CCS obtained on candidate ion structures generated upon MD simulations, description of the gas phase ion structures may be afforded at the molecular level. , The IMS/MD combination requires that the MD parameters and the IMS calibration are adequately set up, and elegant studies on protein ions, synthetic polymers and dendrimers , are reported.…”

Section: Introductionmentioning

confidence: 99%

“…21 By comparing the measured collision cross sections (CCS) with theoretical CCS obtained on candidate ion structures generated upon MD simulations, description of the gas phase ion structures may be afforded at the molecular level. 21,22 The IMS/MD combination requires that the MD parameters and the IMS calibration are adequately set up, and elegant studies on protein ions, 23 synthetic polymers 24 and dendrimers 25,26 are reported. However, Gabelica et al demonstrated that gaseous DNA ions are often characterized by more compact structures than in solution, which are not reproduced using MD simulations when the starting point is the fully desolvated canonical double-helix conformation.…”

Section: ■ Introductionmentioning

confidence: 99%

Structural Characterization of Dendriplexes In Vacuo: A Joint Ion Mobility/Molecular Dynamics Investigation

Saintmont

Hoyas

Rosu

et al. 2022

J. Am. Soc. Mass Spectrom.

Self Cite

View full text Add to dashboard Cite

The combination between ion mobility mass spectrometry and molecular dynamics simulations is demonstrated for the first time to afford valuable information on structural changes undergone by dendriplexes containing ds-DNA and low-generation dendrimers when transferred from the solution to the gas phase. Dendriplex ions presenting 1:1 and 2:1 stoichiometries are identified using mass spectrometry experiments, and the collision cross sections (CCS) of the 1:1 ions are measured using drift time ion mobility experiments. Structural predictions using Molecular Dynamics (MD) simulations showed that gas-phase relevant structures, i.e., with a good match between the experimental and theoretical CCS, are generated when the global electrospray process is simulated, including the solvent molecule evaporation, rather than abruptly transferring the ions from the solution to the gas phase. The progressive migration of ammonium groups (either NH4 + from the buffer or protonated amines of the dendrimer) into the minor and major grooves of DNA all along the evaporation processes is shown to compact the DNA structure by electrostatic and hydrogen-bond interactions. The subsequent proton transfer from the ammonium (NH4 + or protonated amino groups) to the DNA phosphate groups allows creation of protonated phosphate/phosphate hydrogen bonds within the compact structures. MD simulations showed major structural differences between the dendriplexes in solution and in the gas phase, not only due to the loss of the solvent but also due to the proton transfers and the huge difference between the solution and gas-phase charge states.

show abstract

Gas‐phase structure of polymer ions: Tying together theoretical approaches and ion mobility spectrometry

Cited by 7 publications

References 170 publications

Development of Novel Analytical Methods Based on Liquid Chromatography and Electrophoresis

Development of Novel Analytical Methods Based on Liquid Chromatography and Electrophoresis

Elucidation of Dithiol-yne Comb Polymer Architectures by Tandem Mass Spectrometry and Ion Mobility Techniques

Structural Characterization of Dendriplexes In Vacuo: A Joint Ion Mobility/Molecular Dynamics Investigation

Contact Info

Product

Resources

About