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Advanced oxidation technologies for the pulp industry: An investigation on the delignifying properties of the carbonate radical anion
KTH, Superseded Departments, Chemistry.
2004 (English)Doctoral thesis, comprehensive summary (Other scientific)
Place, publisher, year, edition, pages
Stockholm: KTH , 2004. , 90 p.
Series
Trita-KKE, ISSN 0349-6465 ; 0402
Keyword [en]
Chemistry, chemistry, radiation, industrial engineering
Keyword [sv]
Kemi
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-69ISBN: 91-7283-893-0 (print)OAI: oai:DiVA.org:kth-69DiVA: diva2:14676
Public defence
2004-12-08, kollegiesalen, Valhallavägen 79, Stockholm, 09:00
Opponent
Supervisors
Note
QC 20100812Available from: 2004-12-20 Created: 2004-12-20 Last updated: 2010-08-12Bibliographically approved
List of papers
1. Reactivity of the carbonate radical anion towards carbohydrate and lignin model compounds
Open this publication in new window or tab >>Reactivity of the carbonate radical anion towards carbohydrate and lignin model compounds
2003 (English)In: Journal of wood chemistry and technology, ISSN 0277-3813, E-ISSN 1532-2319, Vol. 23, no 1, 47-69 p.Article in journal (Refereed) Published
Abstract [en]

The kinetic selectivity for the reaction of the carbonate radical anion towards lignin and carbohydrate model compounds was determined by pulse radiolysis in the pH-span 8-13. For the cellulose model compound methyl-β-D-glucopyranoside a pKA-value of 14.4 was estimated.

Keyword
Bleaching, Carbonate radical anion, Pulp, Selectivity, electron reduction potentials; phenoxyl radicals; rate constants; peroxynitrite; cations; dioxide; water; chemistry; acidity; damage
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-5265 (URN)10.1081/WCT-120018615 (DOI)
Note
QC 20100812Available from: 2005-06-02 Created: 2005-06-02 Last updated: 2017-12-04Bibliographically approved
2. Reactivity of the Carbonate Radical Anion Towards Carbohydrate and Lignin Model Compounds
Open this publication in new window or tab >>Reactivity of the Carbonate Radical Anion Towards Carbohydrate and Lignin Model Compounds
2003 (English)In: 12th international symposium on wood and pulping chemistry, University of Wisconsin, madison, June 9-12, 2003: Proceedings, vol 1, oral presentations, 2003, 85-87 p.Conference paper, Published paper (Other academic)
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-24067 (URN)
Note
QC 20100812Available from: 2010-08-12 Created: 2010-08-12 Last updated: 2010-08-12Bibliographically approved
3. Peroxynitrite mediated delignification of pulp: A comparative study on the bleaching properties of the carbonate and hydroxyl radicals
Open this publication in new window or tab >>Peroxynitrite mediated delignification of pulp: A comparative study on the bleaching properties of the carbonate and hydroxyl radicals
2004 (English)In: Journal of wood chemistry and technology, ISSN 0277-3813, E-ISSN 1532-2319, Vol. 24, no 2, 83-98 p.Article in journal (Refereed) Published
Abstract [en]

Oxygen delignified pulps were bleached with hydroxyl and carbonate radicals produced from peroxynitrite. The carbonate radical treated pulps showed better selectivity and an increase in brightness. For both radicals, good kappa reductions were obtained. This study shows that the carbonate radical anion is a possible green oxidant for future delignification technologies.

Keyword
Delignification, Hydroxyl and carbonate radicals, Kappa, viscosity, and brightness values, Peroxynitrite
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-5270 (URN)10.1081/WCT-200026553 (DOI)000223809300001 ()2-s2.0-4544345768 (Scopus ID)
Note
QC 20100812Available from: 2005-06-02 Created: 2005-06-02 Last updated: 2017-12-04Bibliographically approved
4. The Carbonate Radical as One-Electron Oxidant of Carbohydrates in Alkaline media
Open this publication in new window or tab >>The Carbonate Radical as One-Electron Oxidant of Carbohydrates in Alkaline media
2005 (English)In: Holzforschung, ISSN 0018-3830, E-ISSN 1437-434X, Vol. 59, no 2, 143-146 p.Article in journal (Refereed) Published
Abstract [en]

The mechanism by which the carbonate radical anion reacts with D-glucose in alkaline aqueous solutions has been studied by means of gamma-radiolysis. From the product analysis it is concluded that the reaction sequence is initiated by a one-electron transfer between the carbonate radical anion and deprotonated D-glucose. In the presence of molecular oxygen, the major, if not only products of this reaction sequence are formic acid, arabinose and gluconic acid and reaction schemes are proposed to account for the observed formation of these products.

Keyword
carbonate radical, deprotonated glucose, one-electron transfer, beta-scission, 1, 2 H-shift
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-5266 (URN)10.1515/HF.2005.021 (DOI)000227384700006 ()2-s2.0-14844314191 (Scopus ID)
Note
QC 20100812Available from: 2005-06-02 Created: 2005-06-02 Last updated: 2017-12-04Bibliographically approved
5. A comparative study on the degradation of cotton linters induced by carbonate and hydroxyl radicals generated from peroxynitrite
Open this publication in new window or tab >>A comparative study on the degradation of cotton linters induced by carbonate and hydroxyl radicals generated from peroxynitrite
2005 (English)In: Holzforschung, ISSN 0018-3830, E-ISSN 1437-434X, Vol. 59, no 2, 132-142 p.Article in journal (Refereed) Published
Abstract [en]

Carbonate (CO3.(-)) and hydroxyl (HO.) radicals were chemically produced in cotton linter suspensions using peroxynitrite as a radical precursor. Both radicals could degrade cotton linters, as shown by viscosity and GPC-SEC measurements. As evidenced by the viscosity measurements, the presence of oxygen during the cotton linter treatments slightly increased cellulose degradation by both radicals. For the carbonate radical, more than 90% of the viscosity losses could be recovered by reductive NaBH4 treatment before measuring the viscosity, whereas only approximately 40% of the viscosity was recovered after hydroxyl radical degradation and subsequent NaBH4 treatment. This indicates that carbonate radicals mainly abstract H-atoms adjacent to hydroxyl groups, i.e., at C-2, C-3 and C-6. This intramolecular selectivity may reflect a polar effect, whereby hydrogen atom abstractions from these positions are favoured. In addition, abstraction at C-6 would be sterically and statistically favoured.

Keyword
carbonate radical; cellulose; cotton linters; degradation; fibre; hydroxyl radical; intramolecular selectivity; peroxynitrite; pulse-radiolysis; hydrogen-peroxide; aqueous-solution; pernitrous acid; nitric-oxide; decomposition; oxidations; homolysis; peroxonitrite; chemistry
National Category
Chemical Process Engineering
Identifiers
urn:nbn:se:kth:diva-5269 (URN)10.1515/HF.2005.020 (DOI)000227384700005 ()2-s2.0-14844313731 (Scopus ID)
Note
QC 20100812Available from: 2005-06-02 Created: 2005-06-02 Last updated: 2017-12-04Bibliographically approved

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