ࡱ> v F ? @ A d e 3 4  > ? @ x V W X w d8F?Ԗ?־ll i 5NO߸dRL}THuU!3oMeؔgh$QӭMXt~/VaD̷1/;m5NтfT<ϨBT@ Q!* D: /u _p'0BT@ Q!* DBT@ Q!* DBT@ Q!* DBT@ Q!* DBT@ Q!* DBT@ Q!* DBT@ Q!* DBT@ Q!* DBT@ Q!* DBT@ Q!* DBT@ Q!* DBT@ Q!* DBT@ Q!* DBT@  nIENDB`rDd\C  c AD:\MATKO\magistarski rad\PHB-ATBC\10 deg-min-svi uzorci-engl.bmpbpqs~4Dd Lq&nDqs~4Dd PNG  IHDR d.gAMAPLTEٟ pHYs+ IDATx_{ur,Z.rC*k*^Vq?.b7b/(po4T^&pTe3䎛f'") &2l5;T^9THERMAL DEGRADATION OF POLY(3-HYDROXYBUTYRATE) PLASTICIZED WITH ACETYL TRIBUTYL CITRATE Matko ERCEG, Branka ANDRI I, Tonka KOVA I & Ivka KLARI Department of Organic Chemical Technology, Faculty of Chemical Technology, University of Split, Teslina 10/V, 21 000 Split, Croatia E-mail: baric@ktf-split.hr Abstract The effects of acetyl tributyl citrate (ATBC) as biodegradable plasticizer for poly(3-hydroxybutyrate) were studied by the differential scanning calorimetry (DSC) and by the thermogravimetric method under dynamic conditions in inert atmosphere. The thermal degradation of plasticized PHB samples was investigated as a function of annealing temperature, annealing time and cooling rate after the thermal treatment. The amounts of ATBC varied from 10% to 30%. From the data obtained it can be concluded that Key words: thermal degradation, DSC, thermogravimetry, poly(3-hydroxybutyrate), acetyl tributy citrate, plasticizer 1. Introduction Poly(3-hydroxybutyrate) (PHB) is fully biodegradable thermoplastic with biocompatibility and ecological safety produced by a wide variety of bacteria [1,2]. Therefore, it has much potential, among other applications, as biodegradable plastics. However, until now there is no large commercial production of PHB products because PHB has higher cost, narrow processability window and brittleness than commercial polymers. To replace commodity polymers in packaging film materials film extrusion of the PHB has to be performed what is a difficult process because of PHB's brittleness and thermal instability. Among the other routes to prepare useful material from PHB, the addition of plasticizers contributes to improve the polymer thermal and mechanical properties. Plasticizers for PHB, as biodegradable polymer, should preferably also be biodegradable, because in case of packaging formed by different components, some of which are compostable and some are not, the packaging as a whole is not compostable [3]. Furthermore, non of the conventional polyolefin stabilizers gives any significant improvement in the stability of PHB [4]. For food packaging and hygiene applications, only non-toxic substances can be considered as plasticizers. Citrate plasticizers are derived from naturally occurring citric acid. They are non-toxic and are used as plasticizers with some biodegradable polymers [5,6]. In this work we used acetyl tributyl citrate (ATBC) as PHB plasticizer. 2. Experimental part Materials The materials used in this study were poly(3-hydroxybutyrate) (Biomer, Germany) and acetyl tributyl citrate (Merck KgaA, Germany). The plasticized samples containing 1030 wt.% of acetyl tributyl citrate were prepared by depositing the plasticizer on PHB powder surface from ethanol solution. The mixture was thoroughly stirred and the solvent was evaporated. The powdered mixture was compression molded at 160C for 5 s and cut to small pieces. This step was repeated three times to insure sample homogeneity before the final compression molding at 170C for 15 s. Experimental Conditions DSC measurements were performed on a Perkin-Elmer DSC-4 differential scanning calorimeter with Model 3600 Data Station (TADS) under nitrogen atmosphere (30 cm3/min). The investigations were performed under following conditions: The effect of annealing temperature: the samples were heated from 50C to various annealing temperatures (180-220C) at heating rate of 40C/min, kept at annealing temperature for 10 min, than cooled to 50C at 40C/min. The second run was registered (heating rate 10C/min). The effect of annealing time: the annealing temperature of 190C was chosen. The heating and cooling conditions remained the same as described in a), only the annealing time was varied (0, 5, 10, 20 and 40 min). The second scan was registered. The effect of cooling rate: the samples were heated from 50C to 200C at the heating rate 40C/min and annealed for 10 min. The samples were cooled down at different cooling rates (40, 10 and 5C/min) to 50C. The second scan was registered (heating rate 10C/min, from 50C to 200C). The thermal degradation of the plasticized PHB (mass 6,8 0,5 mg) was carried out thermogravimetrically in the temperature range from 50 to 450C using a Perkin-Elmer TGS-2 system with Model 3600 Data Station. The nitrogen flow rate was 30 cm3/min and the heating rates were 2.5, 5, 10 and 20C/min. 3. Results and discussion The changes in DSC thermograms for pure PHB and for PHB with 20 wt.% of ATBC due to annealing for 10 min at various temperatures are shown in Figures 1(a) and (b), respectively.  Figure 1. DSC thermograms of pure PHB (a) and PHB+20%ATBC (b) at different annealing temperatures. For pure PHB the position of the highest maximum is almost the same for 180 and 190C, but for higher temperature values it is shifted towards lower temperatures. For pure PHB at 190C appearance of a small shoulder can be observed. The maximum of the peak annealed at higher temperatures is located approximately at the same temperature as the shoulder at lower temperature. Furthermore, the addition of ATBC shifts position of the highest peak to lower temperatures while the shapes of the curves are similar to those of pure PHB. The effect of time of annealing at 190C on the shape of thermograms for pure PHB and for PHB with 20 wt.% of ATBC is shown in Figures 2(a) and (b), respectively.  Figure 2. DSC thermograms of pure PHB (a) and PHB+20%TBAC (b) at different annealing times. KOMENTIRATI KAD SNIMI It is known that changes of the thermogram shape may occur not only as a result of thermal degradation but also due to a different thermal history of the sample. Therefore, the various cooling rates were applied (40C/min, 10C/min and 5C/min). The effect of cooling rate after thermal treatment on the shape of DSC thermograms for pure PHB and for PHB with 20 wt.% of ATBC is shown in Figures 3(a) and (b), respectively.  Figure 3. DSC thermograms of pure PHB (a) and PHB+20%TBAC (b) at different cooling rates. It is evident that rate of cooling influence the shape of DSC thermograms. Decrease in the cooling rate leads to increase of the height of the shoulder and decrease of the height of the main peak. This effect is the most pronounced for pure PHB. With addition of ATBC heights of both shoulders and main peaks decrease. Furthermore, the positions of the peaks are shifted to lower temperatures. The non-isothermal thermogravimetric (TG) curves of pure PHB and PHB with addition of ATBC obtained in the temperature range 50-650C at the heating rates of 2,5C/min and corresponding derivative thermogravimetric (DTG) curves are shown in Figure 4(a) and (b), respectively. Figure 4. TG (a) and corresponding DTG (b) curves of non-isothermal degradation of pure PHB and PHB with 10, 20 and 30 wt.% of ATBC. 4. Conclusions References M. J. Pettinari, G. J. Vasquez, D. Silberschmidt, B. Rehm, A. Steinbuchel, B. S. Mendez: Applied and Environmental Microbiology, (2001), 5331-5334. J. Riesmeier, J. Koman, R. Trethewey, A. Heyer, V. Landschtze, L. Willmitzer: Polymer Degradation and Stability, 59 (1998) 383-386. EN 13432:2000. Requirements for packaging recoverable through composting and biodegradation test scheme and evaluation criteria for the final acceptance of packaging. N. Grassie, E. J. Murray: Polymer Degradation and Stability, 6 (1984) 127-134. L. V. Labrecque, R. A. Kumar, V. Dave, R. A. Gross, S. P. McCarthy: Journal of Applied Polymer Science, 66 (1997) 1507-1513. 9GR-Gsyon>ya(0JVB4 i@Ҁ$IH$! HB4 i@Ҁ$IH$! HB4 i@Ҁ$IH$! HB4 i@Ҁ$IH$݂FLoJ4"uW&4$Nv??فV4ʲ>}CHO^1p !GO]$r|v\|=c~{h4&*EHҿ`a߾Fo¶?(M̾O*g睶?,7+??.<'l*{_}ao_g>~{Dz ']_[jjywxg 9: 9 & F$&(34=>9: 9+)*D\qzupkfa;>  8 X  M   b F^_t%+)*D\q25-. ! & F & F$ & Fq25-. !""_#`#a#b#ĿR    J     d op #ѭi5{c}\uwnpG-Ҁ e߲o>~YP ,Ƴȝg<}~$Hi̬-hT&,IH$%'Hc^o@Ҁ?1FӘҀ%IH$! 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Yu. A. Trotsenko, L. L. Belova: Microbiology, 69 No. 6 (2000) 753-763. V. P. Ghiya, V. Dave, R. A. Gross and S. P. McCarthy: Pure Appl. Chem. 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This effect is more pronounced for pure PHB than for From the data obtained PHB and to 30%.temperatures are shown in FiguresFig.and broadens the thermograms.The effect of timeFig. It is obvious that the degradation is more pronounced for longer degradation times for all samples indicated by broadening the curves and by their shift to lower temperatures. This is more pronounced for samples containing ATBC than for pure PHB.ig. 3. DSC thermograms of purein peak. This effect is more pronounced for pure PHB than for The dynamicsFig. From the DSC measurements it can be concluded that thermal degradation of poly(3-hydroxybutyrate) proceeds rapidly above 190. The rate of degradation is increasing with increasing the annealing temperature and the annealing time. Addition of ATBC accelerates the thermal degradation of PHB and therefore ATBC can't be used in order to improve thermal properties of PHB. 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U jU jU jejU j'U jHtU jU jU jU jOU5mH 5 jKUmH  jkUmH mH : 2\t@K! ٨aG!]4VI@\UK93 o\NtCbh9Ii~#'g|e|q[{R-o!?@XL թ`h$MÔ6~ׇ2|C‡}y%f/ gXK QjPYy,G|R@46J/>Z ֶТLҤ^qUz dc@9/^I-z!5g`q).5 G IDATZiR0 4C;Pgq}ȏwǗ6ԁMZb^qda[抗$qw6rS_K)LX@iAIxJ ϝ-5bg5{O yij6r\D~!Pl+R=$);Du؊a[PHB and to 30%. temperatures are shown in FiguresFig.and broadens the thermograms.The effect of timeFig. It is obvious that the degradation is more pronounced for longer degradation times for all samples indicated by broadening the curves and by their shift to lower temperatures. This is more pronounced for samples containing ATBC than for pure PHB.ig. 3. DSC thermograms of purein peak. This effect is more pronounced for pure PHB. The dynamicsFig.A changes neither nor the residual weight at the end of this degradation step, but it slightly lowers the maximal rate of degradation. From the DSC measurements it can be concluded that thermal degradation of poly(3-hydroxybutyrate) proceeds rapidly above 190. The degradation is accelerated by addition of ATBC what is indicated by broadening the thermograms and by their shift to lower temperatures. From the dynamic TG measurements it can be concluded that the thermal degradation of pure and plasticized PHB is very rapid and it occurs through one degradation step. The addition of ATBC leads to earlier start of thermal degradation. Therefore, ATBC can't be used to improve thermal properties of PHB. m, A. Steinbuchel, B. S. Mendez,, V. Landschtze, L. Willmitzer,Yu. A. Trotsenko, L. L. Belova, (6) N. Grassie, E. J. Murray,ve, R. A. Gross, S. P. McCarthy,, d]}dfYĝ$Fmbk6E]GRـ4stB TچEri~o m%ڷ멿Ieu@J!:lG$t-r ;*@d.|Hlb[?x؛@B nEOH\\q(w @,><vbP D!%)508>R@QU R9,Uu\,,aanB Y݅Vsmcuh)d4-R.W7wn};4, K¶1@b=a^XOrv]$%ݻ٘Eu{EZb;e˲%{U5ι+ a!M_|@WWHys՞ %?oδ:>ĮlH@oXHk).HiIo8ms}T -*N !fM S}u ü [$@$NormalmH 4@4 Heading 1$@&5CJ<A@<Default Paragraph Font.B@. 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E-mail address: merceg PHB and to 30%. temperatures are shown in FiguresFig.and broadens the thermograms.The effect of timeFig. It is obvious that the degradation is more pronounced for longer degradation times for all samples indicated by broadening the curves and by their shift to lower temperatures. This is more pronounced for samples containing ATBC than for pure PHB.ig. 3. DSC thermograms of purein peak. This effect is more pronounced for pure PHB. The dynamicsFig.A changes neither nor the residual weight at the end of this degradation step, but it slightly lowers the maximal rate of degradation. From the DSC measurements it can be concluded that thermal degradation of poly(3-hydroxybutyrate) proceeds rapidly above 190. The degradation is accelerated by addition of ATBC what is indicated by broadening the thermograms and by their shift to lower temperatures. From the dynamic TG measurements it can be concluded that the thermal degradation of pure and plasticized PHB is very rapid and it occurs through one degradation step. The addition of ATBC leads to earlier start of thermal degradation. Therefore, ATBC can't be used to improve thermal properties of PHB. m, A. Steinbuchel, B. S. 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