| 1. |
- Andersson, M., et al.
(författare)
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Size and structure characterization of ethylhydroxyethyl cellulose by the combination of field-flow fractionation with other techniques. Investigation of ultralarge components
- 2004
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Ingår i: Biomacromolecules. - : Wiley. - 1525-7797 .- 1526-4602. ; 5:1, s. 97-105
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Tidskriftsartikel (refereegranskat)abstract
- Ethylhydroxyethyl cellulose (EHEC) of three different viscosity classes (EHEC I, II, and III) was analyzed by programmed cross-flow asymmetrical flow field-flow fractionation coupled to multiangle light scattering and refractive index detectors to determine their size and molar mass distribution. Two size populations were detected in the two lower viscosity classes, EHEC I and II, one high molar mass and one ultrahigh molar mass (UHM). The two covered molar masses from 10(4) up to 10(9) g.mol(-1). The highest viscosity class EHEC III was less size-dispersed covering molar masses from 5x10(5) to 5x10(7) g.mol(-1). Filtering of the EHEC II solution removed small amounts of compact UHM material. Enzyme treatments were performed on EHEC II to further characterize it. Matrix-assisted laser desorption/ionization time-of-flight mass spectrometry and anion ion-exchange chromatography coupled to pulsed amperometric detection showed that the UHM component contained EHEC.
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| 2. |
- Andersson, M, et al.
(författare)
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Size and Structure Characterization of Ethylhydroxyethyl Cellulose by the Combination of Field-Flow Fractionation with Other Techniques. Investigation of Ultralarge Components
- 2004
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Ingår i: Biomacromolecules. - : American Chemical Society (ACS). - 1526-4602 .- 1525-7797. ; 5:1, s. 97-105
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Tidskriftsartikel (refereegranskat)abstract
- Ethylhydroxyethyl cellulose (EHEC) of three different viscosity classes (EHEC I, II, and III) was analyzed by programmed cross-flow asymmetrical flow field-flow fractionation coupled to multiangle light scattering and refractive index detectors to determine their size and molar mass distribution. Two size populations were detected in the two lower viscosity classes, EHEC I and II, one high molar mass and one ultrahigh molar mass (UHM). The two covered molar masses from 104 up to 109 g·mol-1. The highest viscosity class EHEC III was less size-dispersed covering molar masses from 5 × 105 to 5 × 107 g·mol-1. Filtering of the EHEC II solution removed small amounts of compact UHM material. Enzyme treatments were performed on EHEC II to further characterize it. Matrix-assisted laser desorption/ionization time-of-flight mass spectrometry and anion ion-exchange chromatography coupled to pulsed amperometric detection showed that the UHM component contained EHEC.
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| 3. |
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| 4. |
- Enebro, Jonas, 1979-, et al.
(författare)
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A New Approach for Studying Correlations between the Chemical Structure and the Rheological Properties in Carboxymethyl Cellulose
- 2007
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Ingår i: Biomacromolecules. - : American Chemical Society (ACS). - 1525-7797 .- 1526-4602. ; 8:10, s. 3253-3257
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Tidskriftsartikel (refereegranskat)abstract
- Two model sodium carboxymethyl celluloses (CMC) with similar monomer composition but with significant differences in the viscoelastic properties, that could not be assigned to variations in the average molar mass or molar mass distribution, were investigated with respect to the fraction of nonsubstituted cellulose segments in the polymers. The CMCs were hydrolyzed by a purified highly selective endoglucanase. The average molar mass and molar mass distribution of the enzyme products, as measured by size-exclusion chromatography with online multi-angle light scattering and refractive index detection (SEC/MALS/RI), revealed that the enzyme-catalyzed hydrolysis was more effective on one of the CMCs. To investigate whether this was due to a higher fraction of nonsubstituted cellulose segments in the polymer, the concentrations of nonsubstituted enzyme products, e.g., cellotetraose and cellopentaose, were measured by matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOFMS). It was concluded that the two CMCs displayed significant differences in the fraction of nonsubstituted cellulose segments. Furthermore, the CMC with the strongest attractive intermolecular interactions, according to rheometry, also contained the highest fraction of nonsubstituted cellulose segments.
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| 5. |
- Enebro, Jonas, 1979-, et al.
(författare)
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Investigation of endoglucanase selectivity on carboxymethyl cellulose by mass spectrometric techniques
- 2009
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Ingår i: Cellulose. - : Springer Science and Business Media LLC. - 0969-0239 .- 1572-882X. ; 16:2, s. 271-280
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Tidskriftsartikel (refereegranskat)abstract
- The benefits of applying cellulose selective enzymes as analytical tools for chemical structure characterization of cellulose derivatives have been frequently addressed over the years. In a recent study the high selectivity of cellulase Cel45A from Trichoderma reesei (Tr Cel45A) was utilized for relating the chemical structure to the flow properties of carboxymethyl cellulose (CMC). However, in order to take full advantage of the enzymatic hydrolysis the enzyme selectivity on the cellulose substrate must be further investigated. Therefore, the selectivity of Tr Cel45A on CMC was studied by chemical sample preparation of the enzyme products followed by mass spectrometric chemical structure characterization. The results strongly suggest that, in accordance with recent studies, also this highly selective endoglucanase is able to catalyze hydrolysis of glucosidic bonds adjacent to mono-substituted anhydroglucose units (AGUs). Furthermore, the results also indicate that substituents on the nearby AGUs will affect the hydrolysis.
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| 6. |
- Enebro, Jonas, 1979-, et al.
(författare)
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Liquid Chromatography combined with Mass Spectrometry for the Investigation of Endoglucanase Selectivity on Carboxymethyl Cellulose
- 2009
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Ingår i: Carbohydrate Research. - : Elsevier BV. - 0008-6215 .- 1873-426X. ; 344:16, s. 2173-2181
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Tidskriftsartikel (refereegranskat)abstract
- Endoglucanases are useful tools in the chemical structure analysis of cellulose derivatives. However, knowledge on the endoglucanase selectivity, which is of central importance for data interpretation, is still limited. In this study, new reverse-phase liquid chromatography mass spectrometry (LC-MS) methods were developed to investigate the selectivity of the endoglucanases Cel5A, cel7B, Cel45A, and Cel74A from the filamentous fungus Trichoderma reesei. The aim was to improve the identification of the regioisomers in the complex mixtures that are obtained after enzymatic hydrolysis. Reduction followed by per-O-methylation was performed in order to improve the separation in reverse-phase LC, increase MS sensitivity, and to facilitate structure analysis by MS/MS of O-carboxymethyl glucose and cellooligosaccharides. The cellulose selective enzymes that were investigated displayed interesting differences in enzyme selectivity on CMC substrates.
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| 7. |
- Enebro, Jonas, 1979-
(författare)
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New Mass Spectrometric Methods for Structure Analysis of Carboxymethyl Cellulose
- 2008
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Carboxymethyl cellulose (CMC) is a cellulose derivative, made from cellulose by introduction of carboxymethyl groups along the molecules. The properties of CMC are affected by several parameters where the molar mass and molar mass distribution, degree of substitution (DS) and the distribution pattern along, and between, the cellulose molecules are the most prominent. In the present thesis we have investigated the use of various mass spectrometric techniques, such as matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOFMS) and electrospray ionization MS (ESI-MS), for characterization of the chemical structure of CMC. We here present a refined sample preparation procedure for MALDI that greatly facilitates the spectrum acquisition and improves the quality of the mass spectrum when analyzing partially hydrolyzed CMC. The refined method allows for estimation of the DS in CMC samples as a complement to more expensive and laborious methods. We also show that by combining MALDI-TOFMS with selective hydrolysis, by purified endoglucanase, and size-exclusion chromatography (SEC) it is possible to differentiate between CMCs of similar monomer composition but differences in the substitution pattern. Our findings show that the CMC containing longer non-substituted cellulose segments along the polymer backbone also displayed the highest intermolecular interactions in solution, as measured by rheometry. In order to take full advantage of the selective hydrolysis, provided by purified endoglucanases, more information regarding their selectivity on CMC must be investigated. We therefore present methods where chemical sample preparation of the oligomeric enzyme products is performed in order to facilitate the chemical structure characterization by ESI-MS/MS and liquid chromatography MS (LC-MS). These methods provides valuable information regarding the substituent distribution along the oligomeric enzyme products, and thereby gives indications regarding the selectivity of the endoglucanases on CMC substrates. From our finding we are able to present interesting information regarding the selectivity of four endoglucanases (Cel7B, Cel5A, Cel45A and Cel74A) from the filamentous fungus Trichoderma reesei and provide plausible explanations to their apparent differences in selectivity on CMC.
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| 8. |
- Kaali, Peter, et al.
(författare)
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Antimicrobial properties of Ag+ loaded zeolite polyester polyurethane and silicone rubber and long-term properties after exposure to in-vitro ageing
- 2010
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Ingår i: Polymer degradation and stability. - : Elsevier BV. - 0141-3910 .- 1873-2321. ; 95:9, s. 1456-1465
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Tidskriftsartikel (refereegranskat)abstract
- In biomedical applications, tubes (e.g. catheters etc.) are commonly produced from polyurethane (PU) and silicone rubber which are known to be biocompatible materials. Several studies have shown that tubes, which are connected to the body (invasive) (especially urinary, tracheotomy and central venous catheters) are associated with infections. The present study reports the development of a new method aiming at obtaining antibacterial properties for PU and silicone rubber by mixing respective material with a natural antibacterial agent (Ag+ loaded zeolite) in different weight fractions. The influence of the zeolite content on the antimicrobial properties were analysed by exposure to bacteria (ISO 22196) and mixtures of fungi (ISO 846). The materials were also subject to artificial body fluids (Artificial Lysosomal Fluid (ALF) and Gamble's solution) for periods up to three months and the subsequent changes in the chemical properties after in-vitro exposure were determined by Matrix Assisted Laser Deposition/Ionization Time Of Flight Mass Spectrometry (MALDI-TOF MS) and Attenuated Total Reflection Fourier Transform Infra Red spectroscopy (ATR-FTIR). It was established that the antimicrobial effect of the materials increased with the increase of the zeolite content. The wettability of the materials was found to decrease significantly during the in-vitro exposure, but this could not be correlated to the zeolite content. In the PU samples, the formation of free carbonyl and -OH groups was observed, which corresponds to oxidative degradation. In case of the silicone rubber the ratio of cyclic PDMS to linear PDMS (H, CH3 and dimethyl terminated) decreased, which indicates a change in the concentration of the compounds. The formation and increase of the O-H bond during the exposure was also confirmed by the infrared spectra of the material which corresponds to hydrolysis of the silicone rubber.
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| 9. |
- Kaali, Peter, et al.
(författare)
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Degradation of Biomedical Polydimethylsiloxanes During Exposure to In Vivo Biofilm Environment Monitored by FE-SEM, ATR-FTIR, and MALDI-TOF MS
- 2010
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Ingår i: Journal of Applied Polymer Science. - : Wiley. - 0021-8995 .- 1097-4628. ; 115:2, s. 802-810
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Tidskriftsartikel (refereegranskat)abstract
- Polymers used for biomedical purposes in medical devices are usually requested to be inert to degradation. This article describes that slow irreversible changes were observed in silicone surfaces exposed to in vivo biofilms even if silicone, in general, is supposed to have excellent long-term properties. Tracheostomy tubes made of silicone rubber were exposed to in vivo biofilm environments in clinical tests for periods of 7, 3, and 6 months. The chemical degradation was monitored by MALDI-TOF MS, ATR-FTI.R, and FE-SEM. In addition, the physical changes were monitored by contact angle and hardness measurements. Cyclic polydimethylsiloxane (PDMS) was detected on the surfaces of new (unaged) silicones. On the surfaces of the in vivo samples new compounds, presumably linear methyl-hydroxyl-terminated PDMS, were detected in addition to cyclic PDMS. These compounds may be formed as a result of the hydrolysis of linear dimethyl terminated PDMS, which is also present in the silicone rubber. ATR-FTIR spectroscopy confirmed that hydrolysis had indeed occurred during the in vivo exposure, since Si-OH groups were detected. Furthermore, significant changes in the topography were detected by FE-SEM, indicating the initiation of degradation. No significant changes in the contact angle of the in vivo used samples were observed, but this information may be shielded by the fact that biofilm may remain on the surface, despite the thorough cleaning before the analysis. It is also possible that the surface hydrophobicity was recovered by the diffusion of linear low-molecular-weight compounds from the bulk.
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| 10. |
- Karlsson, J., et al.
(författare)
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Enzymatic degradation of carboxymethyl cellulose hydrolyzed by the endoglucanases Cel5A, Cel7B, and Cel45A from Humicola insolens and Cel7B, Cel12A and Cel45Acore from Trichoderma reesei
- 2002
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Ingår i: Biopolymers. - : Wiley. - 0006-3525 .- 1097-0282. ; 63:1, s. 32-40
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Tidskriftsartikel (refereegranskat)abstract
- Enzymatic hydrolysis of carboxymethyl cellulose (CMC) has been studied with purified endoglucanases Hi Cel5A (EG II), Hi Cel7B (EG I), and Hi Cel45A (EG V)from Humicola insolens, and Tr Cel7B (EG I), Tr Cel12A (EG III), and Tr Cel45Acore (EG V)from Trichoderma reesei. The CMC, with a degree of substitution (DS) of 0.7, was hydrolyzed with a single enzyme until no further hydrolysis was observed. The hydrolysates were analyzed for production of substituted and non substituted oligosaccharides with size exclusion chromatographly (SEC) and with matrix-assisted laser desorption/ionization mass spectrometry (MALDI-TOF-MS). Production of reducing ends and of nonsubstituted oligosaccharides was determined as well. The two most effective endoglucanases for CMC hydrolysis were Hi Cel5.A and Tr Cel7B. These enzymes degraded CMC to lower molar mass fragments compared with the other endoglucanases. The products had the highest DS determined by MALDI-TOF-MS. Thus, Hi Cel5A and Tr Cel7B were less inhibited by the substituents than the other endoglucanases. The endoglucanase with clearly the lowest activity on CMC was Tr Cel45Acore. It produced less than half of the amount of reducing ends compared to Tr Cel7B; furthermore, the products had significantly lower DS. By MALDI-TOF-MS, oligosaccharide with different degree of polymerization (DP) and with different number of substituents could be separated and identified. The average oligosaccharide DS as function of DP could be measured for each enzyme after hydrolysis. The combination of techniques for analysis of product formation gave information on average length of unsubstituted blocks of CMC.
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