References of "De Pauw, Edwin"
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See detailGas-Phase Dynamics of Collision Induced Unfolding, Collision Induced Dissociation, and Electron Transfer Dissociation-Activated Polymer Ions
Haler, Jean ULiege; Massonnet, Philippe ULiege; Far, Johann ULiege et al

in Journal of the American Society for Mass Spectrometry (in press)

Polymer characterizations are often performed using mass spectrometry (MS). Aside from MS and different tandem MS (MS/MS) tech- niques, ion mobility–mass spectrometry (IM-MS) has been recently added to ... [more ▼]

Polymer characterizations are often performed using mass spectrometry (MS). Aside from MS and different tandem MS (MS/MS) tech- niques, ion mobility–mass spectrometry (IM-MS) has been recently added to the inventory of char- acterization technique. However, only few studies have focused on the reproducibility and robust- ness of polymer IM-MS analyses. Here, we per- form collisional and electron-mediated activation of polymer ions before measuring IM drift times, collision cross-sections (CCS), or reduced ion mobilities (K0). The resulting IM behavior of different activated product ions is then compared to non-activated native intact polymer ions. First, we analyzed collision induced unfolding (CIU) of precursor ions to test the robustness of polymer ion shapes. Then, we focused on fragmen- tation product ions to test for shape retentions from the precursor ions: cation ejection species (CES) and product ions with m/z and charge state values identical to native intact polymer ions. The CES species are formed using both collision induced dissociation (CID) and electron transfer dissociation (ETD, formally ETnoD) experiments. Only small drift time, CCS, or K0 deviations between the activated/formed ions are observed compared to the native intact polymer ions. The polymer ion shapes seem to depend solely on their mass and charge state. The experiments were performed on three synthetic homopolymers: poly(ethoxy phosphate) (PEtP), poly(2-n-propyl- 2-oxazoline) (Pn-PrOx), and poly(ethylene oxide) (PEO). These results confirm the robustness of polymer ion CCSs for IM calibration, especially singly charged polymer ions. The results are also discussed in the context of polymer analyses, CCS predictions, and probing ion–drift gas interaction potentials. [less ▲]

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See detailAnalytical tool for lipopeptide identification
Mc Cann, Andréa ULiege; Kune, Christopher ULiege; Far, Johann ULiege et al

Conference (2018, November 30)

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See detailCombination of Capillary Electrophoresis and Ion mobility coupled to Mass Spectrometry and Theoretical Calculations for cysteine connectivity identification in peptides bearing two intra-molecular disulfide bonds
Delvaux, Cédric ULiege; Massonnet, Philippe ULiege; Kune, Christopher ULiege et al

Conference (2018, November 06)

Disulfide bonds are post translational modification playing essential roles in the biological activity and stability of numerous peptides and proteins. Intra-molecular disulfide bonds are found in various ... [more ▼]

Disulfide bonds are post translational modification playing essential roles in the biological activity and stability of numerous peptides and proteins. Intra-molecular disulfide bonds are found in various natural-occurring peptides such as animal venoms. In such peptides, the appropriate cysteine connectivity provides the required conformation for efficient binding to their molecular targets, which ensures their bioactivity. The characterization of cysteine pairing is still a challenging issue in the analysis of peptides targeting pharmaceutical or pharmacological utilizations. Thus, the use of sensitive, robust and efficient characterization techniques to access the cysteine pairing is crucial. In our workflow,the separation of the disulfide isomers of three peptides bearing two intra-molecular disulfide bonds but different cysteine connectivities have been tested using Capillary Zone Electrophoresis (CZE) and Ion Mobility (IM) coupled to Mass Spectrometry (MS). Results show that CZE-MS and IM-MS act as complementary techniques to unambiguously determine the cysteine connectivity of a given peptide. Indeed, the combination of the relative migration time to a reference peptide in CZE-MS, the drift time in IM-MS and the generation of fragments by Collision Induced Dissociation (CID) led to the attribution of the disulfide connectivities in all studied cases. Finally, theoretical calculations were performed to model the different structures in gas phase and solution, supporting the experimental observations on the basis of the predicted physicochemical properties. [less ▲]

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See detailEffectiveness and limitations of computational chemistry and mass spectrometry in the rational design of target‐specific shift reagents for ion mobility spectrometry
Kune, Christopher ULiege; Haler, Jean ULiege; Far, Johann ULiege et al

in Chemphyschem: A European Journal of Chemical Physics and Physical Chemistry (2018)

Ion mobility spectrometry (IMS) is a gas‐phase separation technique based on ion mobility differences in an electric field. It is largely used for the detection of specific ions such as small molecule ... [more ▼]

Ion mobility spectrometry (IMS) is a gas‐phase separation technique based on ion mobility differences in an electric field. It is largely used for the detection of specific ions such as small molecule explosives. IMS detection system includes the use of e.g. a Faraday plate or mass spectrometry (MS). The presence of interfering ion signals in standalone IMS may lead to the detection of false positives or negatives due to e.g. lacking resolving power. In this case, selective mobility shifts obtained using shift reagents (SR), i.e. ligands complexing a specific target, can bring help. The effectiveness of an SR strategy relies on the SR‐target ion selectivity. The crucial step lies in the SR design. The aim of this paper is to present an efficient interplay of experimental ion mobility mass spectrometry (IMMS) and predictive computational chemistry using various levels of computational efforts for rationally designing target‐specific SR. Mass spectrometry is used to evaluate the efficiency of the SR selectivity with identification and semi‐quantification of free and complexed ions. Minimal computational efforts allow the design of the SR, predict the SR‐target ion relative stabilities, and prediction of ion mobility shifts. We demonstrate our approach using crown ethers and β‐cyclodextrin to selectively shift interfering perchlorate, amino acids and diaminonaphthalene isomers. We also release the software ParsIMoS for straightforward use of ion mobility calculator IMoS. [less ▲]

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See detailMass spectrometry based techniques for lipopeptides analysis
Mc Cann, Andréa ULiege; Delvaux, Cédric ULiege; Far, Johann ULiege et al

Conference (2018, July 05)

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See detailMetallic nanoparticles: an interesting option for mass spectrometry imaging of small molecules in tissues
Verdin, Alexandre ULiege; Müller, Wendy; Bertrand, Virginie ULiege et al

Poster (2018, July 05)

MALDI mass spectrometry imaging is a central technique for the visualisation and identification of a wide variety of molecules in biological samples, especially in tissues slides. However, organic ... [more ▼]

MALDI mass spectrometry imaging is a central technique for the visualisation and identification of a wide variety of molecules in biological samples, especially in tissues slides. However, organic matrices used for the desorption and ionisation of molecules suffers from major limitations, particularly for the analysis of small molecules due to interferences from the matrix in the low m/z range. In this preliminary study we compared the performances of 9-aminoacridine, a well known organic matrix used for small molecules anaylsis, and metallic nanoparticles to evaluate the information obtained from both method. Ionisation by nanoparticles is known as Surface-Assisted Laser Desorption Ionisation (SALDI). Metallic nanoparticles seem to be a promising substrate for MS analysis of small compounds in tissues and reveals information that are complementary to those obtained by MALDI. [less ▲]

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See detailResolving Poly(2-oxazoline) Side Chain Isomers using Tandem Mass Spectrometry and Ion Mobility-Mass Spectrometry
Haler, Jean ULiege; de la Rosa, Victor R.; Massonnet, Philippe ULiege et al

Poster (2018, July 05)

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See detailIon mobility mass spectrometry for lipopeptides analysis
Mc Cann, Andréa ULiege; Delvaux, Cédric ULiege; Far, Johann ULiege et al

Scientific conference (2018, July 04)

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See detailMicroproteomic profiling og high-grade squamous intraepithelial lesions of the cervix
Pottier, Charles ULiege; Kriegsmann, Mark; Smargiasso, Nicolas ULiege et al

Poster (2018, June 06)

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See detailRevisiting protomers of aniline by high-resolution ion mobility spectrometry, capillary electrophoresis-mass spectrometry, and abinitio calculations
Kune, Christopher ULiege; Delvaux, Cédric ULiege; Haler, Jean ULiege et al

Poster (2018, June 05)

The detection of two stable tautomers of protonated aniline, the amino-protonated and the protonated carbone in para position (“Cpara-protonated”), are already reported in the literature. The use of ... [more ▼]

The detection of two stable tautomers of protonated aniline, the amino-protonated and the protonated carbone in para position (“Cpara-protonated”), are already reported in the literature. The use of traveling wave ion mobility spectrometry (TWIMS) spotlights a possible conversion between both of these tautomers. Moreover, the presence of phenol strongly suggests that water adduct(s) is/are involved during this tautomerisation. The use of high resolution ion mobility - mass spectrometry also suggests tautomers conversion and the presence of other metastable species of protonated aniline than the Cpara-protonated and amino-protonated aniline. These observations support that the measurement of protomers ratio should be affect by gas phase reactions. Aqueous and non-aqueous capillary electrophoresis results show the effect of the solvents. The rate of tautomers conversion seems to be higher in protic solvent (water) than aprotic solvent (acetonitrile). [less ▲]

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See detailResolving Poly(2-oxazoline) Side Chain Isomers using Tandem Mass Spectrometry and Ion Mobility-Mass Spectrometry
Haler, Jean ULiege; de la Rosa, Victor R.; Massonnet, Philippe ULiege et al

Poster (2018, June 05)

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See detailInterpreting the global shape of ions by geometric analysis using Ion Mobility-Mass Spectrometry and data fitting
Haler, Jean ULiege; Far, Johann ULiege; de la Rosa, Victor R. et al

Poster (2018, June 04)

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See detailProteomic analysis of osteoblasts secretome provides new insights in mechanisms underlying osteoarthritis subchondral bone sclerosis
Sanchez, Christelle ULiege; Mazzucchelli, Gabriel ULiege; Comblain, Fanny et al

in Annals of the Rheumatic Diseases (2018, June), 77(supplement 2), 894

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See detailCan we correlate ion mobility mass spectrometry data with native solution structures? A crosslinking approach
Hanozin, Emeline ULiege; Grifnée, Elodie ULiege; Morsa, Denis ULiege et al

Poster (2018, June)

Introduction: The structural characterization of biomolecules is of prime importance in the understanding of biological processes at the molecular level. In this context, the development of soft ... [more ▼]

Introduction: The structural characterization of biomolecules is of prime importance in the understanding of biological processes at the molecular level. In this context, the development of soft ionization techniques, namely electrospray ionization, and the advent of ion mobility (IM) separation tools open new perspectives for the analysis of large intact molecular ions by mass spectrometry (MS). Previous (IM-)MS experiments emphasized that the solution phase structures may be (partially) preserved in the gas phase under soft ionization conditions. However, several factors (e.g. coulombic interactions, accelerating voltages) have an influence on the conformation of biomolecular ions in the gas phase and should be carefully considered. Consequently, some fundamental questions remain elusive: “Can we correlate ion mobility mass spectrometry data to native solution structures?” Methods: To bring innovative answers to these longtime debated questions, we here propose an early stage study targeting constrained “native-like” conformations in the gas phase. To this end, we capitalize on a crosslinking approach to establish chemical links between lysine residues located in close spatial proximity within the protein. The so-created covalent network is here used as a scaffold to prevent the collapsing and unfolding of biomolecular ions once desolvated in the gas phase. These “frozen” native solution conformations are then interrogated using ion mobility as implemented on the commercial SYNAPT G2 HDMS spectrometer. Preliminary data: Practically, we used cytochrome c as a model system that we crosslinked with BS3 linkers. Using ion mobility, we monitored the evolution of the collision cross section (CCS) quantity, a rotationally averaged 2D projection of the ion conformation, for each charge state as function of the number of covalent intramolecular linkers. These data were readily compared with those obtained in similar conditions for the non-crosslinked cytochrome c as well as with a benchmark corresponding to the native solution conformations as resolved by NMR spectroscopy. Our results highlight that the crosslinked cytochrome c adopts more compact conformations in the gas phase, closer to values monitored for the native solution conformation, compared to its non-crosslinked homologue. In addition, we found that a critical number of intramolecular linkers were required to prevent structural unfolding from Coulomb repulsions. Novel aspect: Bring innovative answers to the longtime debated native MS questions based on an alternative application of intramolecular covalent linkers. [less ▲]

Detailed reference viewed: 36 (12 ULiège)
See detailThe knotty phenotype of the frd3 Arabidopsis mutant
Scheepers, Maxime ULiege; Spielmann, Julien ULiege; Boulanger, Madeleine ULiege et al

Poster (2018, May 17)

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See detailEvaluation of capillary electrophoresis separation of cyclic lipopeptides
Mc Cann, Andréa ULiege; Far, Johann ULiege; De Pauw, Edwin ULiege et al

Poster (2018, March 29)

Detailed reference viewed: 51 (23 ULiège)