Journal of Polymers and the Environment, Vol. 11, No. 2, April 2003 (© 2003)
1566-2543/03/0400-0039/0 © 2003 Plenum Publishing Corporation
39
1
Swedwood Latvia Ltd., Planupes iela 24, LV-2141 Incukalns,
Latvia.
2
Man-Technology-Environment Research Centre, Örebro University,
SE-701 82 Örebro, Sweden.
3
IFM-Department of Chemistry, University of Linköping,
Linköping, Sweden.
4
To whom all correspondence should be addressed. E-mail: jessika.
hagberg@nat.oru.se
Alkaline Degradation of Cellulose: Mechanisms and Kinetics
Ivars Pavasars,
1
Jessika Hagberg,
2,4
Hans Borén,
3
and Bert Allard
2
Cellulose powder and softwood sawdust were subjected to alkaline degradation under condi-
tions representative of a cementitious environment for periods of 7 and 3 years, respectively.
During the first 3 years, sampling was frequent, and data on the degradation of cellulose and
production of isosaccharinic acid was used for establishing long-term prediction models. Samples
after an additional period of 4 years were compared to the predicted values. The total rate of
degradation was measured as the increase in total organic carbon (TOC) in corresponding so-
lutions. A previously published theoretical model of degradation kinetics gave a good approxi-
mation of the present experimental data. Peeling-off, stopping, and alkaline hydrolysis reaction
rate constants were obtained as model parameters, and the results suggested that the transfor-
mation of the glucose end group is the rate-limiting step in the cellulose peeling-off reaction
and also determines the pH dependence of that reaction. After 3 years, isosaccharinic (ISA) acid
represented 70–85% of all degradation products as quantified by capillary zone electrophore-
sis. The long-term prediction model indicated that all of the cellulose would be degraded after
only 150–550 years. The control sampling after 7 years points toward a lower degradation of
cellulose and production of ISA than predicted by the model, reflecting either a degradation of
ISA that was faster than the production or a termination of the ISA production.
KEY WORDS: Alkaline degradation of cellulose; isosaccharinic acid; prediction models.
INTRODUCTION
Cellulose loses weight upon reaction with alkali,
which is a phenomenon that is well known from pulp-
ing and textile industries [1, 2]. Alkaline degradation
of cellulose has also been studied in relation to trans-
formation of biomass to various low-molecular-weight
products [3, 4]. Thus examinations of alkaline degra-
dation of cellulose have been focused on conditions that
are pertinent for the relevant technological processes,
particularly elevated temperatures.
Alkaline degradation of cellulose is a process of
potential importance in the design and performance
assessment of facilities for long-term disposal of radio-
active waste [5, 6]. Substantial amounts of organic mat-
ter, including cellulose materials such as wood and
paper, can be present in low- and intermediate-level
radioactive wastes [7]. Cementitious facilities have
been proposed for storage of such waste. The highly
alkaline cement pore water in such an environment
would eventually lead to a partial degradation of any
cellulose present. This would lead to a production of
water-soluble, low-molecular-weight species with
metal complexing properties leading to higher solubil-
ity and possibly enhanced mobility of radionuclides in
the deposit.