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Mass spectrometric studies of cellulose ethers

Momcilovic, Dane LU (2005)
Abstract
Cellulose based derivatives, such as cellulose ethers, today find many applications in a diverse range of



fields. The numerous applications put high demands on the technological performance of the cellulose ethers.



In order to be able to control the technological properties it is necessary to develop analytical methods by,



which they can be correlated to the chemical structure. In some cases variations in the technological



properties cannot be explained by the chemical characterisation methods available today. Thus, it is of high



importance to investigate the suitability of new analytical techniques for chemical characterisation of

... (More)
Cellulose based derivatives, such as cellulose ethers, today find many applications in a diverse range of



fields. The numerous applications put high demands on the technological performance of the cellulose ethers.



In order to be able to control the technological properties it is necessary to develop analytical methods by,



which they can be correlated to the chemical structure. In some cases variations in the technological



properties cannot be explained by the chemical characterisation methods available today. Thus, it is of high



importance to investigate the suitability of new analytical techniques for chemical characterisation of



cellulose ethers.



In this thesis matrix-assisted laser desorption/ionisation mass spectrometry (MALDI-MS) and nanoelectrospray



ionisation (nano-ESI)-MS were studied as analytical techniques for cellulose ethers. Among the



results, MALDI tandem mass spectrometry (MS/MS) and nano-ESI-MS/MS were demonstrated as



exceptionally useful tools for the structure analysis of cellulose ether oligosaccharides. Nano-ESI-MS/MS



was employed to characterise the selectivity of a cellulose depolymerising enzyme, endoglucanase, on



methyl cellulose (MC). Novel dialkylamine derivatives of cellulose ether oligosaccharides were shown to



increase the sensitivity in both MALDI- and nano-ESI-MS, and to facilitate structure analysis by MS/MS.



Studies of the molar mass distribution of partially depolymerised MC were performed by size-exclusion



chromatography semi-online to MALDI-MS. The sample preparation method for MALDI was found to have



a significant influence on the outcome of the analysis. Furthermore, a simple experiment showed that, the



combination of MALDI-MS and partial acidic depolymerisation could be used to distinguish between



cellulose ethers of different degrees of substitution. (Less)
Abstract (Swedish)
Popular Abstract in Swedish

Cellulosa etrar är en grupp ämnen som har många tillämpningar inom olika områden. Det stora antalet tillämpningar ställer höga krav på de teknologiska egenskaperna hos cellulosa etrarna. För att kunna kontrollera de teknologiska egenskaperna är det nödvändigt att utveckla analytiska metoder, med vilka egenskaperna kan korreleras till den kemiska strukturen. Ibland går det inte att förklara variationer i de teknologiska egenskaperna med dagens befintliga analysmetoder och tekniker. Därför är det viktigt att undersöka lämpligheten hos nya analytiska tekniker för kemisk karakterisering av cellulosa etrar.



I den här avhandlingen har matris-assisterad laser desorptions/joniserings... (More)
Popular Abstract in Swedish

Cellulosa etrar är en grupp ämnen som har många tillämpningar inom olika områden. Det stora antalet tillämpningar ställer höga krav på de teknologiska egenskaperna hos cellulosa etrarna. För att kunna kontrollera de teknologiska egenskaperna är det nödvändigt att utveckla analytiska metoder, med vilka egenskaperna kan korreleras till den kemiska strukturen. Ibland går det inte att förklara variationer i de teknologiska egenskaperna med dagens befintliga analysmetoder och tekniker. Därför är det viktigt att undersöka lämpligheten hos nya analytiska tekniker för kemisk karakterisering av cellulosa etrar.



I den här avhandlingen har matris-assisterad laser desorptions/joniserings masspektrometri (MALDI-MS) och nano-elektrosprej joniserings masspektrometri (nano-ESI-MS) studerats i syfte att analysera cellulosa etrar. Båda teknikerna har visat sig vara utmärkta verktyg för strukturanalys av oligomerfragment utav cellulosa etrar. Nano-ESI-MS har också använts för att studera selektiviteten hos ett cellulosanedbrytande enzym, endoglukanas, på metyl cellulosa (MC). Då oligomerfragmenten derivatiserades med dialkylaminer kunde det konstateras att känsligheten i MALDI-MS och nano-ESI-MS ökade markant. Dessa derivaten förenklade också för strukturanalys med hjälp av tandem masspektrometri. Molmassefördelningen hos partiellt depolymeriserad MC kunde mätas genom att sammankoppa storleksuteslutningskromatografi med MALDI-MS. Vidare demonstrerades det att det med MALDI-MS mycket enkelt och snabbt går att särskilja cellulosa etrar med olika substitutionsgrad. (Less)
Please use this url to cite or link to this publication:
author
supervisor
opponent
  • Prof. Dr. Mischnick, Petra, Technische Universität Carolo-Wilhelmina zu Braunschweig, Institut für Lebensmittelchemie, Braunschw
organization
publishing date
type
Thesis
publication status
published
subject
keywords
Polymerteknik, biopolymers, Polymer technology, Analytisk kemi, Analytical chemistry, enzymatic depolymerisation, reductive amination, electrospray ionisation, cellulose ethers, MALDI, mass spectrometry
pages
140 pages
publisher
Analytical Chemistry, Lund University
defense location
Lecture Hall B, Centre for Chemistry and Chemical Engineering, Getingevägen 60, Lund, Sweden.
defense date
2005-04-29 10:30:00
ISBN
91-628-6316-9
language
English
LU publication?
yes
additional info
The information about affiliations in this record was updated in December 2015. The record was previously connected to the following departments: Analytical Chemistry (S/LTH) (011001004)
id
30e5d7ea-8677-40ae-ba47-61a036e516fd (old id 544661)
date added to LUP
2016-04-04 11:08:19
date last changed
2018-11-21 21:02:54
@phdthesis{30e5d7ea-8677-40ae-ba47-61a036e516fd,
  abstract     = {{Cellulose based derivatives, such as cellulose ethers, today find many applications in a diverse range of<br/><br>
<br/><br>
fields. The numerous applications put high demands on the technological performance of the cellulose ethers.<br/><br>
<br/><br>
In order to be able to control the technological properties it is necessary to develop analytical methods by,<br/><br>
<br/><br>
which they can be correlated to the chemical structure. In some cases variations in the technological<br/><br>
<br/><br>
properties cannot be explained by the chemical characterisation methods available today. Thus, it is of high<br/><br>
<br/><br>
importance to investigate the suitability of new analytical techniques for chemical characterisation of<br/><br>
<br/><br>
cellulose ethers.<br/><br>
<br/><br>
In this thesis matrix-assisted laser desorption/ionisation mass spectrometry (MALDI-MS) and nanoelectrospray<br/><br>
<br/><br>
ionisation (nano-ESI)-MS were studied as analytical techniques for cellulose ethers. Among the<br/><br>
<br/><br>
results, MALDI tandem mass spectrometry (MS/MS) and nano-ESI-MS/MS were demonstrated as<br/><br>
<br/><br>
exceptionally useful tools for the structure analysis of cellulose ether oligosaccharides. Nano-ESI-MS/MS<br/><br>
<br/><br>
was employed to characterise the selectivity of a cellulose depolymerising enzyme, endoglucanase, on<br/><br>
<br/><br>
methyl cellulose (MC). Novel dialkylamine derivatives of cellulose ether oligosaccharides were shown to<br/><br>
<br/><br>
increase the sensitivity in both MALDI- and nano-ESI-MS, and to facilitate structure analysis by MS/MS.<br/><br>
<br/><br>
Studies of the molar mass distribution of partially depolymerised MC were performed by size-exclusion<br/><br>
<br/><br>
chromatography semi-online to MALDI-MS. The sample preparation method for MALDI was found to have<br/><br>
<br/><br>
a significant influence on the outcome of the analysis. Furthermore, a simple experiment showed that, the<br/><br>
<br/><br>
combination of MALDI-MS and partial acidic depolymerisation could be used to distinguish between<br/><br>
<br/><br>
cellulose ethers of different degrees of substitution.}},
  author       = {{Momcilovic, Dane}},
  isbn         = {{91-628-6316-9}},
  keywords     = {{Polymerteknik; biopolymers; Polymer technology; Analytisk kemi; Analytical chemistry; enzymatic depolymerisation; reductive amination; electrospray ionisation; cellulose ethers; MALDI; mass spectrometry}},
  language     = {{eng}},
  publisher    = {{Analytical Chemistry, Lund University}},
  school       = {{Lund University}},
  title        = {{Mass spectrometric studies of cellulose ethers}},
  year         = {{2005}},
}