Analysis of Multiply Charged Poly(ethylene oxide-co-propylene oxide) Using Electrospray Ionization-Ion Mobility Spectrometry-Mass Spectrometry

Ito, Kanako; Kitagawa, Shinya; Ohtani, Hajime

doi:10.2116/analsci.18p332

Cited by 10 publications

(11 citation statements)

References 23 publications

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“…Indeed, IMS-MS has been extensively used for analyzing multiply charged polymers. [20][21][22][23][24][25][26][27] The molecular distribution of polymers represents another problem for mass spectra interpretation, but the use of MS/MS can limit the distribution to be analyzed. In this case, the first MS selects polymers of a certain m/z range, and the selected ions are analyzed in the second MS after CICS, in which ions attached to the polymers are partially reduced by a relatively soft collision without (or with slight) degradation.…”

Section: Introductionmentioning

confidence: 99%

“…Therefore, IMS can separate ions of the same m/z value but different z value generated from ESI. Indeed, IMS‐MS has been extensively used for analyzing multiply charged polymers 20–27 . The molecular distribution of polymers represents another problem for mass spectra interpretation, but the use of MS/MS can limit the distribution to be analyzed.…”

Section: Introductionmentioning

confidence: 99%

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End group analysis of poly(methylmethacrylate)s using the most abundant peak in electrospray ionization‐ion mobility spectrometry‐tandem mass spectrometry and Fourier transform–based noise filtering

Omae

Ozeki

Kitagawa

et al. 2021

Rapid Comm Mass Spectrometry

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Rationale We recently developed the characterization method for synthetic polymers weighing more than a few tens of kilodalton using electrospray ionization‐ion mobility spectrometry‐tandem mass spectrometry, in which the m/z value of the most abundant peak was used for characterization. However, the identification of the most abundant peak from the isotopic peaks was often difficult due to the background noise. Methods Here, we employed a noise reduction method using Fourier transform (FT) filtering. In the power spectrum obtained using FT of the mass spectrum of the multiple charged analytes, the significant signals in the low‐frequency region and at frequency z are observed for the analytes of z charges. When the signals in both regions were used for inversed FT (i.e., the signals in other regions were zero padded), a noise‐filtered mass spectrum was obtained. Results In the analysis of poly(methylmethacrylate)s weighing 13–17 kDa, mass spectra without noise filtering with relatively high‐intensity noise (than signal) were complicated to identify the most abundant peak. On the contrary, the most abundant peak was clearly identified from the mass spectra after FT‐based noise filtering, and end group composition was estimated successfully. Conclusions The proposed FT‐based noise filtering for the mass spectrum is effective to characterize multiply charged synthetic polymers weighing more than a few tens of kilodalton using electrospray ionization‐ion mobility spectrometry‐tandem mass spectrometry.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

End group analysis of poly(methylmethacrylate)s using the most abundant peak in electrospray ionization‐ion mobility spectrometry‐tandem mass spectrometry and Fourier transform–based noise filtering

Omae

Ozeki

Kitagawa

et al. 2021

Rapid Comm Mass Spectrometry

Self Cite

View full text Add to dashboard Cite

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“…In 2019, Ito et al went a step further by analyzing larger multiply charged PEO, PPO, and PEO- b -PPO- b -PEO copolymers . They probed the influence of the PEO/PPO composition on the IMS response .…”

Section: Introductionmentioning

confidence: 99%

“…Finally, for sufficiently low z / L , all polymer ions adopt a spherical conformation, regardless of their charge. For critical z / L ratios, structural transitions between extended and compact ion shapes are usually witnessed and are evidenced by discontinuities in CCS versus mass evolutions. − In the study on multiply charged homo and copolymers led by Ito, the EO/PO content was shown to play a significant effect on the chain length at which the extended/compact structural transition occurs …”

Section: Introductionmentioning

confidence: 99%

Assessing the Structural Heterogeneity of Isomeric Homo and Copolymers: an Approach Combining Ion Mobility Mass Spectrometry and Molecular Dynamics Simulations

Duez

Moins

Coulembier

et al. 2020

J. Am. Soc. Mass Spectrom.

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Synthetic polymers occupy a unique place in the field of ion mobility mass spectrometry (IMS−MS). Indeed, due to their intrinsic dispersity, they have the asset to offer a broad range of homologous ions with different lengths that can be detected in several charge states. In addition, the gas-phase structure of polymer ions mostly depends on their ability to screen the adducted charges. Several works dealing with linear, cyclic, and star-shaped polymers have already shown that the gas-phase structure of polymer ions heavily relies on the polymer architecture, i.e., the primary structure. In the present work, we move a step further by evaluating whether a relationship exists between the primary and secondary structures of synthetic homo and copolymers. The IMS−MS experiments will be further complemented by MD simulations. To highlight the effectiveness of IMS separation, we selected isomeric homo and copolymers made of lactide (LA) and propiolactone (PL) units. In this way, the mass analysis becomes useless since isomeric comonomer sequences can coexist for any given chain length. An UPLC method was implemented in the workflow to successfully separate all PL−LA comonomer sequences before infusion in the IMS−MS instrument. The analysis of doubly charged copolymers showed that the comonomer sequence has an impact on the IMS response. However, this only holds for copolymer ions with precise sizes and charge states, and this is therefore not a rule of thumb.

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“…[7][8][9][10] Compared with other techniques for characterization of analytes, MS has significant advantages in speed, sensitivity and specificity. [11][12][13][14][15][16] Electrospray ionization (ESI) is one of the soft ionization techniques for MS analysis and ESI-MS has been widely used to characterize protein. 17 Under ESI-MS conditions, a protein molecule is typically detected as multiple-charged ions, and thus charge state distribution (CSD) of protein could be related to protein conformation.…”

Section: Introductionmentioning

confidence: 99%

Direct Detection of Lysozyme in Viscous Raw Hen Egg White Binding to Sodium Dodecyl Sulfonate by Reactive Wooden-tip Electrospray Ionization Mass Spectrometry

Yao

Yuan

et al. 2019

ANAL. SCI.

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Direct characterization of native protein binding to ligands in raw biological samples is a challenging task, because the ligand solution might induce proteins to aggregation, flocculation and denaturation. In this work, we developed a reactive wooden-tip electrospray ionization mass spectrometry (ESI-MS) for formation and characterization of protein-ligand complexes upon rapid mixing in electrospray droplets. Raw viscous hen egg white (HEW) was directly loaded onto a wooden tip to induce spray ionization, and sodium dodecyl sulfonate (SDS) solution was directly loaded into the HEW spray by a pipette tip, and thus lysozyme-DS complexes were then formed in the electrospray droplets and were detected subsequently by mass spectrometry. The new approach was successfully applied to investigate interaction of SDS and native lysozyme in electrospray droplets of standard solution and raw egg white. Our results showed that wooden-tip ESI-MS is a promising method to form and characterize protein-ligand complexes.

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Analysis of Multiply Charged Poly(ethylene oxide-co-propylene oxide) Using Electrospray Ionization-Ion Mobility Spectrometry-Mass Spectrometry

Cited by 10 publications

References 23 publications

End group analysis of poly(methylmethacrylate)s using the most abundant peak in electrospray ionization‐ion mobility spectrometry‐tandem mass spectrometry and Fourier transform–based noise filtering

End group analysis of poly(methylmethacrylate)s using the most abundant peak in electrospray ionization‐ion mobility spectrometry‐tandem mass spectrometry and Fourier transform–based noise filtering

Assessing the Structural Heterogeneity of Isomeric Homo and Copolymers: an Approach Combining Ion Mobility Mass Spectrometry and Molecular Dynamics Simulations

Direct Detection of Lysozyme in Viscous Raw Hen Egg White Binding to Sodium Dodecyl Sulfonate by Reactive Wooden-tip Electrospray Ionization Mass Spectrometry

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