Tandem mass spectrometry and ion mobility mass spectrometry for the analysis of molecular sequence and architecture of hyperbranched glycopolymers.
Identifieur interne : 001555 ( Main/Exploration ); précédent : 001554; suivant : 001556Tandem mass spectrometry and ion mobility mass spectrometry for the analysis of molecular sequence and architecture of hyperbranched glycopolymers.
Auteurs : Xiumin Liu [États-Unis] ; Lydia R. Cool ; Kenneth Lin ; Andrea M. Kasko ; Chrys WesdemiotisSource :
- The Analyst [ 1364-5528 ] ; 2015.
Descripteurs français
- KwdFr :
- MESH :
English descriptors
- KwdEn :
- MESH :
- chemical , chemistry : Polysaccharides.
- methods : Spectrometry, Mass, Electrospray Ionization, Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization, Tandem Mass Spectrometry.
Abstract
Multidimensional mass spectrometry techniques, combining matrix-assisted laser desorption/ionization (MALDI) or electrospray ionization (ESI) with tandem mass spectrometry (MS(2)), multistage mass spectrometry (MS(n)) or ion mobility mass spectrometry (IM-MS), have been employed to gain precise structural insight on the compositions, sequences and architectures of small oligomers of a hyperbranched glycopolymer, prepared by atom transfer radical copolymerization of an acrylate monomer (A) and an acrylate inimer (B), both carrying mannose ester pendants. The MS data confirmed the incorporation of multiple inimer repeat units, which ultimately lead to the hyperbranched material. The various possible structures of n-mers with the same composition were subsequently elucidated based on MS(2) and MS(n) studies. The characteristic elimination of bromomethane molecule provided definitive information about the comonomer connectivity in the copolymeric AB2 trimer and A2B2 tetramer, identifying as present only one of the three possible trimeric isomers (viz. sequence BBA) and only two of the six possible tetrameric isomers (viz. sequences BBA2 and BABA). Complementary IM-MS studies confirmed that only one of the tetrameric structures is formed. Comparison of the experimentally determined collision cross-section of the detected isomer with those predicted by molecular simulations for the two possible sequences ascertained BBA2 as the predominant tetrameric architecture. The multidimensional MS approaches presented provide connectivity information at the atomic level without requiring high product purity (due to the dispersive nature of MS) and, hence, should be particularly useful for the microstructure characterization of novel glycopolymers and other types of complex copolymers.
DOI: 10.1039/c4an01599a
PubMed: 25519163
Affiliations:
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Cool</name></author><author><name sortKey="Lin, Kenneth" sort="Lin, Kenneth" uniqKey="Lin K" first="Kenneth" last="Lin">Kenneth Lin</name></author><author><name sortKey="Kasko, Andrea M" sort="Kasko, Andrea M" uniqKey="Kasko A" first="Andrea M" last="Kasko">Andrea M. Kasko</name></author><author><name sortKey="Wesdemiotis, Chrys" sort="Wesdemiotis, Chrys" uniqKey="Wesdemiotis C" first="Chrys" last="Wesdemiotis">Chrys Wesdemiotis</name></author></titleStmt><publicationStmt><idno type="wicri:source">PubMed</idno><date when="2015">2015</date><idno type="RBID">pubmed:25519163</idno><idno type="pmid">25519163</idno><idno type="doi">10.1039/c4an01599a</idno><idno type="wicri:Area/PubMed/Corpus">001752</idno><idno type="wicri:explorRef" wicri:stream="PubMed" wicri:step="Corpus" wicri:corpus="PubMed">001752</idno><idno type="wicri:Area/PubMed/Curation">001752</idno><idno type="wicri:explorRef" wicri:stream="PubMed" wicri:step="Curation">001752</idno><idno type="wicri:Area/PubMed/Checkpoint">001325</idno><idno type="wicri:explorRef" wicri:stream="Checkpoint" wicri:step="PubMed">001325</idno><idno type="wicri:Area/Ncbi/Merge">000F97</idno><idno type="wicri:Area/Ncbi/Curation">000F97</idno><idno type="wicri:Area/Ncbi/Checkpoint">000F97</idno><idno type="wicri:Area/Main/Merge">001560</idno><idno type="wicri:Area/Main/Curation">001555</idno><idno type="wicri:Area/Main/Exploration">001555</idno></publicationStmt><sourceDesc><biblStruct><analytic><title xml:lang="en">Tandem mass spectrometry and ion mobility mass spectrometry for the analysis of molecular sequence and architecture of hyperbranched glycopolymers.</title><author><name sortKey="Liu, Xiumin" sort="Liu, Xiumin" uniqKey="Liu X" first="Xiumin" last="Liu">Xiumin Liu</name><affiliation wicri:level="2"><nlm:affiliation>Department of Chemistry, The University of Akron, Akron, OH 44325-3601, USA. wesdemiotis@uakron.edu.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>Department of Chemistry, The University of Akron, Akron, OH 44325-3601</wicri:regionArea><placeName><region type="state">Ohio</region></placeName></affiliation></author><author><name sortKey="Cool, Lydia R" sort="Cool, Lydia R" uniqKey="Cool L" first="Lydia R" last="Cool">Lydia R. Cool</name></author><author><name sortKey="Lin, Kenneth" sort="Lin, Kenneth" uniqKey="Lin K" first="Kenneth" last="Lin">Kenneth Lin</name></author><author><name sortKey="Kasko, Andrea M" sort="Kasko, Andrea M" uniqKey="Kasko A" first="Andrea M" last="Kasko">Andrea M. Kasko</name></author><author><name sortKey="Wesdemiotis, Chrys" sort="Wesdemiotis, Chrys" uniqKey="Wesdemiotis C" first="Chrys" last="Wesdemiotis">Chrys Wesdemiotis</name></author></analytic><series><title level="j">The Analyst</title><idno type="eISSN">1364-5528</idno><imprint><date when="2015" type="published">2015</date></imprint></series></biblStruct></sourceDesc></fileDesc><profileDesc><textClass><keywords scheme="KwdEn" xml:lang="en"><term>Polysaccharides (chemistry)</term><term>Spectrometry, Mass, Electrospray Ionization (methods)</term><term>Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization (methods)</term><term>Tandem Mass Spectrometry (methods)</term></keywords><keywords scheme="KwdFr" xml:lang="fr"><term>Polyosides ()</term><term>Spectrométrie de masse ESI ()</term><term>Spectrométrie de masse MALDI ()</term><term>Spectrométrie de masse en tandem ()</term></keywords><keywords scheme="MESH" type="chemical" qualifier="chemistry" xml:lang="en"><term>Polysaccharides</term></keywords><keywords scheme="MESH" qualifier="methods" xml:lang="en"><term>Spectrometry, Mass, Electrospray Ionization</term><term>Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization</term><term>Tandem Mass Spectrometry</term></keywords><keywords scheme="MESH" xml:lang="fr"><term>Polyosides</term><term>Spectrométrie de masse ESI</term><term>Spectrométrie de masse MALDI</term><term>Spectrométrie de masse en tandem</term></keywords></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">Multidimensional mass spectrometry techniques, combining matrix-assisted laser desorption/ionization (MALDI) or electrospray ionization (ESI) with tandem mass spectrometry (MS(2)), multistage mass spectrometry (MS(n)) or ion mobility mass spectrometry (IM-MS), have been employed to gain precise structural insight on the compositions, sequences and architectures of small oligomers of a hyperbranched glycopolymer, prepared by atom transfer radical copolymerization of an acrylate monomer (A) and an acrylate inimer (B), both carrying mannose ester pendants. The MS data confirmed the incorporation of multiple inimer repeat units, which ultimately lead to the hyperbranched material. The various possible structures of n-mers with the same composition were subsequently elucidated based on MS(2) and MS(n) studies. The characteristic elimination of bromomethane molecule provided definitive information about the comonomer connectivity in the copolymeric AB2 trimer and A2B2 tetramer, identifying as present only one of the three possible trimeric isomers (viz. sequence BBA) and only two of the six possible tetrameric isomers (viz. sequences BBA2 and BABA). Complementary IM-MS studies confirmed that only one of the tetrameric structures is formed. Comparison of the experimentally determined collision cross-section of the detected isomer with those predicted by molecular simulations for the two possible sequences ascertained BBA2 as the predominant tetrameric architecture. The multidimensional MS approaches presented provide connectivity information at the atomic level without requiring high product purity (due to the dispersive nature of MS) and, hence, should be particularly useful for the microstructure characterization of novel glycopolymers and other types of complex copolymers. </div></front></TEI><affiliations><list><country><li>États-Unis</li></country><region><li>Ohio</li></region></list><tree><noCountry><name sortKey="Cool, Lydia R" sort="Cool, Lydia R" uniqKey="Cool L" first="Lydia R" last="Cool">Lydia R. Cool</name><name sortKey="Kasko, Andrea M" sort="Kasko, Andrea M" uniqKey="Kasko A" first="Andrea M" last="Kasko">Andrea M. Kasko</name><name sortKey="Lin, Kenneth" sort="Lin, Kenneth" uniqKey="Lin K" first="Kenneth" last="Lin">Kenneth Lin</name><name sortKey="Wesdemiotis, Chrys" sort="Wesdemiotis, Chrys" uniqKey="Wesdemiotis C" first="Chrys" last="Wesdemiotis">Chrys Wesdemiotis</name></noCountry><country name="États-Unis"><region name="Ohio"><name sortKey="Liu, Xiumin" sort="Liu, Xiumin" uniqKey="Liu X" first="Xiumin" last="Liu">Xiumin Liu</name></region></country></tree></affiliations></record>Pour manipuler ce document sous Unix (Dilib)
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