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LETTER COVER
November 4, 2018
Editorial of Polish Journal of Food and Nutrition Sciences (PJFNS)
Department of Chemical and Physical Properties of Food, Institute of Animal Reproduction and Food Research of the Polish Academy of Sciences, Olsztyn, Poland
Dear Editor In Chief of PJFNS,
I am submitting a manuscript for consideration of publication in PJFNS. The manuscript is entitled “Physical, Physicochemical, Chemical, Mechanical and Sensory Properties of Bioplastics From Phosphate Acetylated Arenga Starches”.
It has not been published elsewhere and that it has not been submitted simultaneously for publication elsewhere. We have no conflicts of interest to disclose. Thank you for your consideration of this manuscript.
Sincerely, Abdul Rahim
Departement of Food Science
Faculty of Agriculture, Tadulako University Palu Central Sulawesi, Indonesia.
9/7/2021 Yahoo Mail - New manuscript received by Editorial Office (PJFNS-00284-2019-01)
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From: Polish Journal of Food and Nutrition Sciences ([email protected]) To: [email protected]
Date: Sunday, November 3, 2019, 12:30 PM PST
Dear Dr. Abdul Rahim,
Thank you for submitting your manuscript: Physical, Physicochemical, Mechanical and Sensory Properties of Bioplastics From Phosphate Acetylated Arenga Starches to Polish Journal of Food and Nutrition Sciences
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Polish Journal of Food and Nutrition Sciences
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Physical, Physicochemical, Mechanical and Sensory Properties of Bioplastics From Phosphate Acetylated Arenga Starches
Abdul Rahim1*, Safitri2, Syahraeni Kadir1, Muhardi1, Syamsuddin Laude1, Jusman3 and Steivie Karouw4
1Faculty of Agriculture, Tadulako University,
Jalan Soekarno Hatta Km.9 No.32 Palu, Central Sulawesi, 94118 Indonesia.
2Graduates Faculty of Agriculture, Tadulako University,
Jalan Soekarno Hatta Km. 9 No.32 Palu, Central Sulawesi, 94118 Indonesia
3Faculty of Mathematics and Natural Science, Tadulako University, Jalan Soekarno Hatta Km. 9 No.32 Palu, Central Sulawesi, 94118 Indonesia
4Indonesian Palm Crops Research Institute, Jalan Raya Mapanget PO BOX 1004 Manado Nort Sulawesi, Indonesia.
*Corresponding author, e-mail: [email protected] Telephone: +62451429738, Mobile number: +6285397897809
Abstract
Bioplastics are packaging made from renewable natural materials and have great potential as an alternative to plastic packaging because they do not cause environmental pollution and are easily degraded. The aim of the research was evaluated the physical, physicochemical, mechanical and sensory characteristics of bioplastics from native arenga starch (NAS) and phosphate acetylated arenga starches (PAAS). The PAAS was obtained from the dual modification NAS through acetylation using 5% acetic anhydride and crosslinking using a mixture of sodium trimetaphosphate (STMP) and sodium tripolyphosphate (STPP) (99/1 w/w) with concentrations of 2, 4, 6, 8, 10 and 12% (w/w) of the weight of starch. Thickness, water holding capacity (WHC), oil holding capacity (OHC), water vapor transmission rate (WVTR), water content, biodegradation, tensile strength, elongation, modulus young and sensory properties of the NAS and PAAS bioplastics were investigated. The results showed that the
physicochemical, mechanical and sensory properties of the PAAS bioplastics. The thickness of the NAS and PAAS bioplastics were generally uniform. The WHC of the NAS bioplastic was higher than that of the PAAS. The OHC and WVTR of the PAAS bioplastic increased with the increasing concentration of the STMP/STPP mixture. The water content of the PAAS bioplastics was lower than that of the NAS. Bioplastics weight loss (biodegradation) of the NAS was higher than that of the PAAS and it’s of the PAAS increased with the increasing concentrations of STMP/STPP mixture and bioplastics of the NAS and PAAS can be decomposed completely in the soil. The tensile strength, elongation, modulus young, color and texture of the PAAS bioplastics were better than NAS.
Key words: NAS, PAAS, bioplastics, mixture concentrations of STMP/STPP
INTRODUCTION
The packaging is the final part of the process of producing food or non-food which aims to increase shelf life, consumer acceptance, as a means of supporting the distribution and expansion of product marketing [Prasteen et al., 2018]. The use of the packaging as a packaging material has long been dominated by plastic packaging which increases plastic waste and causes environmental impacts because it is not biodegradable, recycling is quite expensive and contaminated food due to the process of migration of constituent compounds into food ingredients [Ogunrinola & Akpan, 2018]. The solution is to use bioplastics as packaging for food products that are safe and biodegradable.
Bioplastics are packaging made from renewable natural materials and have great potential as an alternative to plastic packaging because they do not cause environmental pollution and are easily degraded. The need for bioplastics has been urgent because the pace of plastic production and air pollution has increased very rapidly. In addition, plastics also cause many health risks because of their toxic nature [Jain & Tiwari, 2015]. Bioplastics are very suitable alternatives to improve the quality of life and maintain a pollution-free planet Earth [Keziah et al., 2018].
Bioplastics made from native starch have poor physicochemical, mechanical, functional and sensory characteristics compared to chemically modified starches. According to Shindu &
and lower solubility compared to native wheat starch. Edible films of acetylated rice starch were stable to heat, a high elongation and rapidly a process of degradation [Collusi et al., 2017]. The mechanical properties of bioplastics from tapioca starch modified using acetic anhydride was better than that the native starch [Tawakaltu et al., 2015]. The elongation, solubility, and oxygen permeability characteristics of biodegradable films from hydroxypropyl sago starch was higher and the water vapor transmission rate was lower than native sago starch [Polnaya et al., 2013].
One of the potential starches to be used as a bioplastic polymer was arenga starch, but native arenga starch has disadvantages such as fast starch retrogradation, cannot stand acidic conditions, low viscosity and paste resistance. These was become reason for starch modification, so that was obtained suitable properties to be applied as a bioplastic polymer materials. The novelty of this research is the use of double modification arenga starch through acetylation and crosslinking as the main raw material in making bioplastic that has not been studied or published.
Phosphate acetylated arenga starch (PAAS) was a dual modified arenga starch through acetylation using acetic anhydride 5% and cross-linking using a mixture of sodium trimetaphosphate (STMP) and sodium tripolyphosphate (STPP) (99/1 w/w) at different concentrations, which has the characteristics of being difficult to retrogradation, stable to heat and acids and resistant to water due to the presence of acetyl groups and cross-linking in the starch molecules. The results of previous studies suggested that the incorporation of acetyl and phosphate in starch molecules were indicates that the retrogradation process inhibited and resistant to heat, acid-base, and water [Rahim et al., 2017]. The objectives of the research was evaluated the physical, physicochemical, mechanical and sensory characteristics of the NAS and PAAS bioplastics through acetylation using 5% acetic anhydride and crosslinked using a mixture of STMP/STPP (99/1 b/b) at different concentrations.
MATERIALS AND METHODS Materials
The materials used in the research consisted of native arenga starch from the pith of palm sugar (Arenga pinnata) trees used in the present work was extracted, distilled water and 98%
acetic anhydride was was purcahsed from Sigma-Aldrich. Hydrochloric acid (HCl) and Sodium
(STPP) (99: 1 w/w), 98% ethanol, glycerol and acetic acid were purchased from Merck (Germany) and other chemicals used was of analytical grade for bioplastic analysis.
Preparation of dual modification arenga starch
Acetylation was carried out according to the method of Rahim et al. [2015] and crosslinking according to the method of Koo et al. [2010] with a slight modification. The suspension consisting of arenga starch (100 g) and distilled water (225 mL) was stirred with a magnetic stirrer for one hour at room temperature. Next 5% (v/w) acetic anhydride was added dropwise until it was finished while maintaining the pH of the suspension from 8.0 to 8.5 by adding 3% NaOH which was carried out at room temperature for 60 minutes. After that the pH was increased to 10.5 by adding 5% NaOH while still stirring, then adding a mixture of STMP/STPP ratio (99: 1 w/w) consisting of 2, 4, 6, 8, 10 and 12% (w/w of the weight of arenga starch) dropwise until finished. Then the suspension was stirred for 30 minutes at room temperature while maintaining a pH of 10.5. The suspension was added to 0.5 N HCl until the pH becomes 4.5 so that the reaction stops. The suspension was deposited for 30 minutes and washed with distilled water three times and ethanol 96% once, then the residue was dried in an oven at 60oC for 15 hours, mashed, and filtered with 100 mesh sieve. Modified arenga starch was obtained PAAS 2, 4, 6, 8, 10 and 12% respectively which were used as bioplastic polymer materials.
Preparation of bioplastics
Bioplastic preparation was carried out according to the method developed by Chung et al.
[2010] with a slight modification. Materials of native arenga starch and PAAS (2, 4, 6, 8, 10 12)% weighed as much as 10 g, then added as much as 150 mL of distilled water, then heated on a hot plate to a temperature of 100oC while stirring. Added 10 mL acetic acid and 3 mL glycerol while still being heated at 100oC. After the solution starts to form a gel, stirrer it for 10 minutes.
The bioplastic solution was poured into stainless steel strips and dried at room temperature for 4 days. The bioplastics obtained were analyzed for their physical, physicochemical, mechanical and sensory properties.
Thickness determination
Bioplastic thickness was measured according to the method [Turhan & Sabhaz, 2004].
Thickness was measured by calipers, by placing bioplastics between the jaws of the caliper.
Thickness was measured at five different places and then the average was calculated.
Water and oil holding capacity determination
The water and oil holding capacity of bioplastic were measured based on a method developed by Larrauri et al. [1996] with some modification. Briefly, 25 mL of distilled water or olive oil were added to 250 mg of bioplastic samples, stirred and left at room temperature for 1 hour. After centrifugation at 3,500 g for 30 minutes, the residue was weighed and the holding capacity of water and oil were calculated as g of water or oil per g of dry bioplastic sample, respectively.
Water vapor transmission rate determination
Water vapor transmission rate (WVTR) was determined using method by Xu et al.
[2005]. Make a saturated salt solution in a chamber by preparing a jar with a diameter of 12 cm and a height of 15 cm and then adjust the humidity (RH) chamber 75% by adding a solution of 40% NaCl (w/v), then stored at room temperature. Acrylic cup (diameter 5 cm and height 1.8 cm) filled with silica gel as much as 10 g, then covered with bioplastic according to the size of the cup. A cup that has been covered with bioplastics was placed in a 75% RH chamber. Water vapor diffused through bioplastics and silica gel will add weight to silica gel. Weighing of the cup along with bioplastics and silica gel was carried out every hour for 8 hours to determine weight gain. The data obtained was made a graph of the relationship between time and weight, then the slope was determined. The WVTR was determined by the equation:
WVTR (g/h/m2) = Change of bioplastics sample weight (g/h) Surface area of the bioplastics sample (m2)
Moisture content determination
Moisture content was measured following the method by AOAC, [2005]. The empty cup was cleaned, then labeled and then heated in the oven at 105oC for 20 minutes, cooled in a desiccator then weighed (W0). Bioplastics of 0.5 g was weighed in a cup and then weighed again
desiccator then weighed until they get a constant value (W2). The moisture content of the bioplastics was obtained through the equation:
Moisture content (%) =WW1 – W2
1 – W0 x 100%
Biodegradability analysis
The biodegradability of bioplastics samples were investigated according the method by Ashok et al. [2018] with slight modification. Bioplastics was cut into 1 cm x 4 cm, buried in the soil at a depth of 8 cm. Curing duration varies for 9 days. Before being buried, the weight of the sample was weighed (W1). Bioplastic samples that had been buried for 9 days were weighed again (W2) and observed changes due to degradation during burial in the soil. Determination of weight loss due to the biodegradation process follows the following formula:
Weight Loss (%) = W1- W2
W1 X 100%
Tensile strength, elongation and modulus young determination
Tensile Strength and elongation were measured using a Mechanical Universal Testing Machine. Bioplastics were cut to standard. The test was carried out by means of the two ends clamped to the testing machine at a speed of 10 mm/minutes, with the distance between the clamps was 50 mm. The start knob was turned on and the tool will pull the sample until it breaks and note the tensile strength and the elongation after breaks. Tensile strength was calculated based on the maximum force (newton) divided by the area of the bioplastic (mm2) applied to the bioplastic until it breaks.
Tensile Strength (MPa) = FMax. (N)
Bioplastic surface area (mm2) The elongation was determined by the equation:
Elongation (%) =Maximum length - Initial length
Initial length x 100%
Modulus young was calculated based on the value of tensile strength and elongation at break Modulus Young (MPa) =Tensile Strength
Elongation/100
Sensory evaluation
The sensory tests of the bioplastics samples were performed using 15 member panel consisted of the adult population (students) of the Faculty of Agriculture, Tadulako University, Central Sulawesi Indonesia. Bioplastics were cut into small pieces and then sensory tests were carried out on the crumb color, texture, aroma and overall acceptability using a hedonic scale. A 7 point hedonic scale were used where 7 - highly very like, 6 - very like, 5 - like, 4 - neither like nor dislike, 3 somewhat like, 2 - dislike and 1 - very dislike. The panelists were instructed to rate the attributes indicating their degree of liking or disliking by putting a number as provided in the hedonic scale according to their preference.
Statistical analysis
Observation data were analyzed by analysis of variance (ANOVA) with one way ANOVA test using SPSS version 22. The means of the results were compared with Duncan’s multiple tests, and the statistical significance was defined at p ≤ 0.05.
RESULTS AND DISCUSSION Thickness
Bioplastic thickness in native arenga starch (NAS) and phosphate acetate arenga starches (PAAS) at different concentrations of STMP/STPP mixture are shown in Figure 1. PAAS bioplastic thickness did not significantly affect at different concentrations of the STMP/STPP mixture. These phenomenon was probably caused the amount of raw material used is equal (10 g), both NAS and PAAS bioplastics. The highest bioplastic thickness of 0.57 mm was obtained in PAAS with a mixture concentration of STMP/STPP 2% and the lowest 0.45 mm was found in PAAS with a concentration of STMP/STPP 8%.
The results showed that the bioplastics obtained had the potential to be made into environmentally friendly plastic bag materials. According to Marichelvam et al. [2019], the average bioplastic thickness of corn starch and rice starch were 0.25 mm and it can be used as biodegradable plastic bags. Ghasemlou et al. [2013] reported that the thickness value of edible
several edible films made from of potato, rice, wheat, gelatin, and sorghum starch having bioplastic film thickness of 0.053 to 0.063 mm.
Water and oil holding capacity
The water and oil holding capacity (WHC, OHC) of bioplastic NAS and PAAS at different concentrations of the STMP/STPP mixture are shown in Figure 2. The WHC and OHC did not significantly on at different concentrations of STMP/STPP mixtures. The highest bioplastics WHC of 33.27 (g/g) was found on NAS and the lowest of 24.19 (g/g) was found on PAAS with a mixture concentrations of STMP/STPP 2%, while the highest bioplastic OHC of 43.45 (g/g) was found on PAAS with a mixture concentration of STMP/STPP 12% and lowest of 30.09 (g/g) was found in PAAS with a mixture concentration of STMP/STPP 6%.
The WHC of the NAS bioplastic was higher than that of the PAAS. It was due to cause by PAAS which has cross-linking bonds in starch molecules to strengthen the modification of starch molecules and prevent water penetration into starch molecules. The WHC of PAAS bioplastic decreases with increasing concentration of the STMP/STPP mixture. The water uptake of bioplastics from cassava peel starch reinforced with microcrystalline cellulose (Avicel PH101fillers) was lower compared to native cassava peel starch. This could be mainly attributed to the strong hydrogen bonds between microcrystalline cellulose and the molecular structure of starch [Maulida et al., 2016]. The OHC of bioplastic has a tendency increased with the increasing concentrations of STMP/STPP mixture. This is presumably due to the presence of hydrophobic acetyl groups and cross-linking can trap oil in modified starch molecules. The results were in accordance with those of the earlier report of Sondari & Iltizam [2018], that the OHC (hydrophobic) of bioplastics from modified cassava starch was lower than that of the native cassava starch.
Water vapor transmission rate
Water vapor transmission rates (WVTR) of the NAS and PAAS bioplastic at different concentrations of the STMP/STPP mixture are given in Figure 3. PAAS bioplastic WVTR significantly affect at different concentrations of the STMP/STPP mixture. The highest bioplastic WVTR of 2.40 g/h/m2 was obtained on NAS and the lowest of 1.05 g/h/m2 was found on PAAS
smaller than that of the NAS. These phenomenon was probably caused the PAAS has a rigid and compact molecular network structure by the presence of cross-linking that can prevent water into the starch molecules. The results were in accordance with those of the earlier report of Detduangchan et al. [2014], that WVTR bioplastic of the modified rice starch was smaller than that native rice starch. Incorporation acetate and crosslinking rice starch as raw materials of bioplastic were reducing WVTR becaused the acetyl group was hydrophobic and crosslinking rice starch was reducing OH groups in the starch molecules [Lόpez et al., 2011].
Fakhoury et al. [2012] reported that WVTR of the native cassava starch film was higher (4.88 g mm/m2 d kPa) compared to acetylated and crosslinked cassava starch (3.59 g mm/m2 d kPa). This phenomenon was caused by the strong interaction between amylose and amylopectin in the modified starch molecules. Bioplastics which have a low WVTR value are suitable for packaging food products to avoid damage caused by the surrounding environment.
Water content
The water content of the NAS and PAAS bioplastic at different concentrations of the STMP/STPP mixture are as can be seen at Figure 4. The PAAS bioplastic water content significantly affect at different concentrations of the STMP/STPP mixture. The highest bioplastic water content of 24.11% was obtained on NAS and the lowest of 21.16% was found in PAAS with a mixture concentration of STMP/STPP 8%. The water content of the PAAS bioplastics was lower than that of the NAS. These was due to caused PAAS has a phosphate group in starch granules that form cross-linking so that the molecular structure more the stable and strongly. In addition, NAS is more hydrophilic than that of the PAAS. The results of the research by Kocakulak et al. [2019] that biofilms made from chickpea flour was added with hydrophilic material (glycerol) will have been higher water content.
According to Gutiérrez et al. [2014] that water content of phosphated corn starch edible film was faund of 30%, whereas water content of native corn starch was obtained of 44%. It was thought that modification of corn starch with STMP increases chemical interactions in starch molecules. Atef et al. [2015] reported that bioplastics was expected to have low water content so that their application as food packaging does not contribute to increasing the amount of water in the product.
Biodegradation
Bioplastic biodegradability testing was carried out using the method sorial burial test to determine the rate of degradation of the bioplastics sample in the soil within a certain time.
Biodegradation can be interpreted as a process of decomposition by microbial activity in the soil, which results in the transformation of the structure of a compound so that changes in molecular integrity occur. Average value of weight loss of the NAS and PAAS bioplastics at different concentrations of the STMP/STPP mixture are achieved in Figure 5. The weight loss (biodegradation) did not significantly the at different concentrations of STMP/STPP mixtures.
The highest bioplastic weight loss of 31.39% was found in NAS and the lowest of 22.15% was obtained in PAAS with a mixture concentration of STMP/STPP 2%.
Bioplastics weight loss of the NAS was higher than that of the PAAS and it’s of the PAAS increased with the increasing concentrations of STMP/STPP mixture. This shows that NAS bioplastics more easily degraded compared to PAAS bioplastics but were not significant.
Biodegradability tests of potato peel bioplastic showed that about 71% of degraded in moist soil within four weeks [Arikan & Bilgen, 2019]. Bioplastics made from native corn and rice starches and modified starches can be biodegradable by the influence of temperature, humidity, and biological activity until 48.73% was achieved within 15 days for bioplastics placed in the soil at a depth of 3 cm [Marchelvam et al., 2019].
Mechanical properties
The mechanical properties of bioplastics measured were tensile strength, elongation and modulus of young. Tensile strength is the magnitude of the force required to achieve maximum pull in each bioplastic area. Elongation is the percentage change in bioplastic length that calculated when bioplastics was pulled up to break. Modulus young is the result of the divided of tensile strength with elongation. The average values of tensile strength, elongation, and modulus young of the NAS and PAAS bioplastics at different concentrations of STMP/STPP mixture are shown in Table 1. Bioplastic tensile strength did not significantly affect at the concentrations of the STMP/STPP mixture, while the elongation and modulus young significantly affect at the concentration of the STMP/STPP mixture.
Tensile strength of the PAAS bioplastic was increased at mixture concentrations of STMP /
showed that the mixture concentrations of STMP / STPP 2 to 6% have been occurred crosslinking that suitable thereby improving the tensile strength of bioplastic to produced.
According to Sartika et al. [2018], the tensile strength of bioplastic avocado seed starch added by microcrystalline cellulose palm fiber was higher than native avocado seed starch. Woggum et al., [2014] suggested that the bioplastic tensile strength of dual modified rice starch with a mixture of STMP 2% - STPP 5% was higher than native rice starch. Starch modified crosslinking is cause increased rigid and compact structure of the starch molecules. Elongation of the NAS bioplastic was smaller than that of the PAAS and elongation of the PAAS bioplastics increased with increasing mixture concentrations of STMP/STPP up to 6% and then constant until the end of 12%. Modulus young of the NAS and PAAS bioplastic was constant for all treatments. The elongation and modulus young of bioplastics from chitosan cross-linking methylcellulose using STMP 0.1 and 0.3% was higher than chitosan bioplastics [Wang et al., 2019].
Sensory attributes
Sensory testing of a product is intended to measure consumer reactions and the level of liking for a product. The average values of crumb color, texture, aroma and overall acceptability of the NAS and PAAS bioplastics at different concentrations of STMP/STPP mixture are given in Table 2. The crumb color and texture of bioplastic significantly influence at concentrations of the STMP/STPP mixture, while the aroma and overall acceptability have no significant effect on the concentration of the STMP/STPP mixture. The crumb colors and texture the PAAS at different concentrations of the STMP/STPP mixture were higher than that of the NAS. This showed that the bioplastic crumb color of the PAAS through acetylation followed by crosslinking with STMP/STPP mixture more transparent compared of the NAS. The color of the bioplastics from oxidized, cross-linked and dual oxidation cross-linked lotus rhizome starch was clearer compared to native lotus rhizome starch [Sukhija et al., 2019].
Texture of the NAS bioplastic was lower than that of the PAAS at different concentrations of STMP/STPP mixture. The texture of bioplastic of dual modified arenga starches have been more smoother surface caused there were cross-linking that made the starch molecules compact arranged. Wang et al., [2019] showed that colors and texture of films made from chitosan methylcellulose crosslinking more transparent and smooth because it was
CONCLUSIONS
Physic, physicochemical, mechanical and sensory properties of bioplastics of at different concentrations of STMP/STPP 2 to 6% was better than that of the NAS. Bioplastics from PAAS has been potential to be applied as food packaging and provide a new alternative to conventional plastic packaging.
ACKNOWLEDGMENT
The author would like to thank the laboratory staffs of Agricultural Processing Technology, Faculty of Agriculture, Tadulako University, Central Sulawesi Indonesia for their useful contributions.
RESEARCH FUNDING
We are grateful to the Ministry of Research, Technology and Higher Education for supporting funding through the Basic Research scheme with Contract Number:
100/SP2H/LT/DRPM/2019 dated March 21, 2019.
CONFLICT OF INTEREST
The authors declare that they have no conflict of interest.
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28. Sukhija, S., Singh, S., Riar, C.S. (2019). Development and characterization of biodegradable films from whey protein concentrate, psyllium husk and oxidized, crosslinked, dual-modified lotus rhizome starch composite. Journal of the Science of Food and Agriculture, 99(7), 3398–3409.
29. Tawakaltu, A.R.A., Egwim, E.C., Ochigbo, S.S., Ossai, P.C. (2015). Effect of acetic acid and citric acid modification on biodegradability of cassava starch nanocomposite films. Journal of Materials Science and Engineering, B 5(9-10), 372-379.
30. Turhan, K.N., Sahbaz, F. (2004). Water vapor permeability, tensile properties and solubility of methylcellulose-based edible film. Journal Food Engineering, 61, 459-466.
31. Wang, H., Liao, Y., Wu, A., Li, B., Qian, J., Ding, F. (2019). Effect of sodium trimetaphosphate on chitosan-methylcellulose composite films: Physicochemical properties and food packaging application. Polymers, 11(2), 368.
32. Woggum, T., Sirivongpaisal, P., Wittaya, T. (2014). Properties and characteristics of dual- modified rice starch based biodegradable films. International Journal of Biological Macromolecules, 67, 490–502.
33. Xu, Y., Miladinov, V., Hanna, M.A. (2004). Synthesis and characterization of starch acetates withhigh substitution. Journal Cereal Chemistry, 81(6), 735-740.
Legends to Figures:
Figure 1. Thickness of bioplastic NAS and PAAS at different concentrations of STMP/STPP mixture.
Figure 2. The WHC and OHC of bioplastics NAS and PAAS at different concentrations of STMP/STPP mixture.
Figure 3. The WVTR of bioplastics NAS and PAAS at different concentrations of STMP/STPP mixture.
Figure 4. Water content of bioplastics NAS and PAAS at different concentrations of STMP/STPP mixture.
Figure 5. Weight loss of bioplastics NAS and PAAS at different concentrations of STMP/STPP mixture.
List of Tables:
Table 1. Average values of tensile strength, elongation, and modulus young of the NAS and PAAS bioplastics at different concentrations of STMP/STPP mixture.
Table 2. Sensory values of the NAS and PAAS bioplastics at different concentrations of STMP/STPP mixture.
Table 1. Average values of tensile strength, elongation, and modulus young of the NAS and PAAS bioplastics at different concentrations of STMP/STPP mixture.
STMP/STPP mixture
Tensile Strength (MPa)
Elongation
(%) Modulus Young (MPa)
NAS 1.08±0.09a 7.03±0.83a 0.15±0.01ab
PAAS 2% 1.10±0.12a 7.87±1.28ab 0.14±0.01ab PAAS 4% 1.09±0.29a 7.78±1.45ab 0.14±0.04ab PAAS 6% 1.16±0.16a 9.14±1.09b 0.13±0.02ab PAAS 8% 0.94±0.07a 8.09±1.05b 0.12±0.01a PAAS 10% 0.93±0.03a 8.17±0.54ab 0.11±0.01a PAAS 12% 0.99±0.11a 7.87±1.17ab 0.13±0.01ab
Data are mean ± standard deviation (SD). Values in the same column with different superscript indicate a significant difference (p<0.05). NAS = Native arenga starch, PAAS = phosphate acetylated arenga starches.
Table 2. Sensory values of the NAS and PAAS bioplastics at different concentrations of STMP/STPP mixture.
STMP/STPP
mixture Crumb color Texture Aroma Overall acceptability NAS 4.60±0.74a 4.60±1.12a 4.48±1.13a 5.33±0.72a PAAS 2% 5.40±0.63b 5.47±0.99b 4.60±0.83a 5.33±0.72a PAAS 4% 5.27±0.88ab 5.53±0.92b 4.73±0.70a 5.53±0.83a PAAS 6% 4.93±0.88ab 5.47±0.99b 4.53±0.64a 5.60±0.63a PAAS 8% 5.67±1.11b 5.27±0.96ab 5.07±0.88a 5.47±0.64a PAAS 10% 5.13±0.99ab 5.20±0.86ab 5.07±0.96a 5.20±0.68a PAAS 12% 5.07±1.03ab 5.13±0.74ab 4.73±1.03a 5.20±0.68a
Data are mean ± standard deviation (SD). Values in the same column with different superscript indicate a significant difference (p < 0.05). NAS = Native arenga starch, PAAS = phosphate acetylated arenga starches.
NAS 2% 4% 6% 8% 10% 12%
Thickness 0.42 0.36 0.41 0.38 0.45 0.37 0.39
0.42
0.36
0.41 0.38
0.45
0.37 0.39
0.0 0.2 0.4 0.6 0.8
NAS 2% 4% 6% 8% 10% 12%
Thickness (mm)
PAAS at Different Concentrations of STMP/STPP Mixture
NAS 2% 4% 6% 8% 10% 12%
WHC 33.27 24.19 24.81 28.16 27.4 26.51 24.49
OHC 30.02 33.76 38.39 35.67 39.92 34.62 43.45
33.27
24.19 24.81
28.16 27.40 26.51
24.49 30.02
33.76
38.39
35.67
39.92
34.62
43.45
0 5 10 15 20 25 30 35 40 45 50
NAS 2% 4% 6% 8% 10% 12%
WHC and OHc (g/g)
PAAS at Different Concentrations of STMP/STPP Mixture
WHC OHC
NAS 2% 4% 6% 8% 10% 12%
WVTR 2.40 1.10 1.05 1.51 1.62 1.66 1.69
2.40c
1.10a
1.05a
1.51ab 1.62b 1.66b 1.69b
0.00 0.50 1.00 1.50 2.00 2.50 3.00
NAS 2% 4% 6% 8% 10% 12%
WVTR (g/h/m2)
PAAS at Different Concentrations of STMP/STPP Mixture
NAS 2% 4% 6% 8% 10% 12%
Water Content 24.11 21.17 22.03 22.25 21.16 21.68 22.15
24.11d
21.17a
22.03bc 22.25c
21.16a 21.68b 22.15bc
15 17 19 21 23 25 27
NAS 2% 4% 6% 8% 10% 12%
Moisture Content (%)
PAAS at Different Concentrations of STMP/STPP Mixture
NAS 2% 4% 6% 8% 10% 12%
Weight Loss 31.39 22.15 24.45 25.68 26.38 28.69 30.29
31.39
22.15 24.45 25.68 26.38 28.69 30.29
0 5 10 15 20 25 30 35 40 45
NAS 2% 4% 6% 8% 10% 12%
Weight Loss (%)
PAAS at Different Concentrations STMP/STPP Mixture
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Physical, Physicochemical, Mechanical and Sensory Properties of Bioplastics From Phosphate Acetylated Arenga Starches
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TITLE AND TYPE
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Title
Physical, Physicochemical, Mechanical and Sensory Properties of Bioplastics From Phosphate Acetylated Arenga Starches
Short title
Bioplastics From Phosphate Acetylated Arenga Starches
Type
Original article
ABSTRACT
2
Bioplastics are packaging made from renewable natural materials and have great potential as an alternative to plastic packaging because they do not cause environmental pollution and are easily degraded. The aim of the research was evaluated the physical, physicochemical, mechanical and sensory characteristics of bioplastics from native arenga starch (NAS) and phosphate acetylated arenga starches (PAAS). The PAAS was obtained from the dual modification NAS through acetylation using 5% acetic anhydride and
crosslinking using a mixture of sodium trimetaphosphate (STMP) and sodium tripolyphosphate (STPP) (99/1 w/w) with concentrations of 2, 4, 6, 8, 10 and 12% (w/w) of the weight of starch. Thickness, water holding capacity (WHC), oil holding capacity (OHC), water vapor transmission rate (WVTR), water content,
biodegradation, tensile strength, elongation, modulus young and sensory properties of the NAS and PAAS bioplastics were investigated. The results showed that the mixture concentrations of STMP/STPP 2 to 6%
have been improved the physic, physicochemical, mechanical and sensory properties of the PAAS bioplastics. The thickness of the NAS and PAAS bioplastics were generally uniform. The WHC of the NAS bioplastic was higher than that of the PAAS. The OHC and WVTR of the PAAS bioplastic increased with the increasing concentration of the STMP/STPP mixture. The water content of the PAAS bioplastics was lower than that of the NAS. Bioplastics weight loss (biodegradation) of the NAS was higher than that of the PAAS and it’s of the PAAS increased with the increasing concentrations of STMP/STPP mixture and bioplastics of the NAS and PAAS can be decomposed completely in the soil. The tensile strength, elongation, modulus young, color and texture of the PAAS bioplastics were better than NAS.
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AUTHORS
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CORRESPONDING AUTHORDr. Abdul Rahim ([email protected])
Food Science, Faculty of Agriculture, Tadulako University, Indonesia
Contribution A - Research concept and design
D - Writing the article
E - Critical revision of the article F - Final approval of the article
Country Indonesia
Phone +6285397897809
ORCID iD ~ 0000-0001-7220-3825
Dr. Safitri Safitri (safi[email protected])
Food Science, Faculty of Agriculture, Tadulako University, Indonesia Contribution B - Collection and/or assembly of data
C - Data analysis and interpretation
Country Indonesia
Phone +6282347698182
ORCID iD ~ 0000-0002-8807-9520
Dr. Syahraeni Kadir ([email protected])
Food Science, Faculty of Agriculture, Tadulako University, Indonesia
Contribution A - Research concept and design
D - Writing the article
F - Final approval of the article
Country Indonesia
Phone +6285228060974
ORCID iD ~ 0000-0003-3727-8404
Dr. Muhardi Muhardi ([email protected])
Agrotechnology, Faculty of Agriculture, Tadulako University, Indonesia Contribution C - Data analysis and interpretation
E - Critical revision of the article
Country Indonesia
Phone +6285396723888
ORCID iD ~ 0000-0003-1630-532X
Dr. Syamsuddin Laude ([email protected])
Agrotechnology, Faculty of Agriculture, Tadulako University, Indonesia
Contribution A - Research concept and design
F - Final approval of the article
Country Indonesia
Phone +62811450095
ORCID iD ~ 0000-0002-1271-3564
Dr. Jusman Jusman ([email protected])
Chemical Science, Faculty of Mathematics and Natural Science, Tadulako University, Indonesia Contribution B - Collection and/or assembly of data
E - Critical revision of the article F - Final approval of the article
Country Indonesia
Phone +6282394780081
Dr. Steivie Karouw ([email protected])
Food Scince Indonesian Palm Crops Research Institute Indonesia
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Food Scince, Indonesian Palm Crops Research Institute, Indonesia Contribution B - Collection and/or assembly of data
D - Writing the article
Country Indonesia
Phone +628124490971
ORCID iD ~ 0000-0003-0796-0832
AUTHOR'S STATEMENTS
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T CHECKEDT CHECKED
T CHECKED
The contents of this manuscript have not been copyrighted or published previously
The contents of the manuscript are not now under consideration for publication elsewhere
Authors are aware of publication fee and agree to pay the fee once the manuscript is accepted for publication
KEYWORDS
5
NAS, PAAS, bioplastics, mixture concentrations of STMP/STPP
MANUSCRIPT CLASSIFICATION
6
Carbohydrates Functional foods Functional properties Packaging
Cereals and Grains
ADDITIONAL INFORMATION
7
Does the manuscript have external funds?
YES
Funding source
The Ministry of Research, Technology and Higher Education for supporting funding through the Basic Research scheme with Contract Number: 100/SP2H/LT/DRPM/2019 dated March 21, 2019.
COVER LETTER
8
LETTER COVER November 4, 2018
Editorial of Polish Journal of Food and Nutrition Sciences (PJFNS)
Department of Chemical and Physical Properties of Food, Institute of Animal Reproduction and Food Research of the Polish Academy of Sciences, Olsztyn, Poland
Dear Editor In Chief of PJFNS,
I am submitting a manuscript for consideration of publication in PJFNS. The manuscript is entitled “Physical, Physicochemical, Chemical, Mechanical and Sensory Properties of Bioplastics From Phosphate Acetylated Arenga Starches”. It has not been published elsewhere and that it has not been submitted simultaneously for publication elsewhere. We have no conflicts of interest to disclose. Thank you for your consideration of this manuscript.
Sincerely, Abdul Rahim
Departement of Food Science
Faculty of Agriculture, Tadulako University Palu Central Sulawesi, Indonesia.
o Cover Letter.pdf (377.62 kB)
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Department of Food Science, Faculty of Food Technology and Agro-industry, Mataram University, Jalan Majapahit No. 62 Mataram Indonesia. (Indonesia)
Prof. Yaya Rukayadi b [email protected]
Department of Food Science, Faculty of Food Science and Technology, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor Darul Ehsan, Malaysia. (Malaysia)
Prof. Yudi Pranoto b [email protected]
Department of Food and Agricultural Technology, Faculty of Agricultural Technology, Gadjah Mada University. Jalan Flora No.1 Bulaksumur, Yogyakarta 55281 Indonesia (Indonesia)
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Manuscript body (1)Manuscript.docx (59.16 kB) Show
Tables (2)
1. Table 1..docx (15.29 kB)
Table 1. Average values of tensile strength, elongation, and modulus young of the NAS and PAAS bioplastics at different concentrations of STMP/STPP mixture.
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2. Table 2..docx (15.43 kB)
Table 2. Sensory values of the NAS and PAAS bioplastics at different concentrations of STMP/STPP mixture. Show
Figures (5)
1. Figure 1..xlsx (12.64 kB)
Figure 1. Thickness of bioplastic NAS and PAAS at different concentrations of STMP/STPP mixture. Show 2. Figure 2..xlsx (15.44 kB)
Figure 2. The WHC and OHC of bioplastics NAS and PAAS at different concentrations of STMP/STPP mixture. Show 3. Figure 3..xlsx (14.29 kB)
Figure 3. The WVTR of bioplastics NAS and PAAS at different concentrations of STMP/STPP mixture. Show 4. Figure 4..xlsx (13.44 kB)
Figure 4. Water content of bioplastics NAS and PAAS at different concentrations of STMP/STPP mixture. Show 5. Figure 5.xlsx (12.56 kB)
Figure 5. Weight loss of bioplastics NAS and PAAS at different concentrations of STMP/STPP mixture. Show
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Authors:
Abdul Rahim, Safitri Safitri, Syahraeni Kadir, Muhardi Muhardi, Syamsuddin Laude, Jusman Jusman, Steivie Karouw
Decision letter:
February 05, 2020 PJFNS-00284-2019-01
Physical, Physicochemical, Mechanical and Sensory Properties of Bioplastics From Phosphate Acetylated Arenga Starches
Dear Dr. Abdul Rahim,
Reviewer and Editor have commented on your paper. You will see that they are advising MAJOR REVISION of your manuscript. Their comments are appended below.
Please revise your paper strictly according to the attached Reviewer's comments.
Your manuscript will not be taken into consideration without the revisions made according to Reviewer's recommendations and without submitted list of changes or a rebuttal against each point which is being raised when you submit the revised manuscript.
Your revision is due by: 2020-02-26
To submit a revision, go to https://www.editorialsystem.com/pjfns/ and log in as an Author. You will see a menu item call Manuscript requires revision. You will find your submission record there.
PLEASE MAKE CHANGES IN COLOR OR IN 'TRACK CHANGES' FUNCTION OF WORD.
Kind regards, Joanna Molga Executive Editor
Polish Journal of Food and Nutrition Sciences Review 1:
The submitted paper deals with the effect of acetylation with acetic anhydride and crosslinking with a mixture of sodium trimetaphosphate and sodium
tripolyphosphate on the selected (barrier against water and oil, mechanical, sensory) properties of the arenga starch materials in the context of their use as packaging materials. In addition, the results of biodegradability tests of these materials are also presented. The data are interesting, however, it seems that the manuscript needs significant correction in terms of the use of English, as in the
PJFNS-00284-2019-01
present form it certainly contains too many mistakes (some sentences are not easy to follow) which make the reading impossible in many places. For example: lines 41-42, lines: 66-68, 74-76, 82-87, 96-97, 101-103, 107, 109, 126-128, 196-197, 202-204, 221-223, 225-227, 241-243, 253, 257, 262-264.
The paper needs also some revision in order to improve its clarity of presentation.
That is why in my opinion, the manuscript needs rewriting.
My suggestions and remarks are listed below.
General remarks:
1. Definition of each acronym (for instance: STMP, STPP) should appear just once, at its first appearance in the text.
2. I do not think there are any significant differences in values presented in Figs 1, 2, and 5. Hence, statistical analysis is needed.
3. As per the requirement of Polish Journal of Food and Nutrition Science, instead of
% concentration of STMP/STPP mixture, the expression such as g/kg, g/L, mg/kg, mg/mL should be used.
4. Instead of ‘modulus young’ and ‘elongation’ there should be ‘Young’s modulus’
and ‘elongation at break’, respectively.
5. The whole Materials subsection is unclear, therefore it should be rewritten. Also, concluding remarks to emphasize the importance of the study are missing.
6. In my opinion, FTIR spectra analysis of bioplastic obtained is needed to show that cross-linking of the starch, which the authors write about, actually took place.
Minor points:
Lines 35-36: What does it mean that ‘The tensile strength, elongation, modulus young, color and texture of the PAAS bioplastics were better than NAS’?
Lines 24: and 29-30: What do the authors mean by ‘functional characteristics’ and
‘better mechanical properties’, respectively? Please clarify.
Lines 140-141: It is stated that ‘The cups with the bioplastics were (…) cooled in a desiccator’. For moisture content determination, keeping bioplastics in an empty desiccator might not be sufficient and true values, not be obtained. Cooling bioplastics with P2O5 would be more appropriate. Please respond to this point.
Lines: 181-182, 209-210, 220, 237, 275-281, 286-89, 298-299: The statistical significance in the differences of data obtained needs to be taken into account.
Lines 184-185: It is stated that ‘The highest bioplastic thickness of 0.57 mm was obtained in PAAS with a mixture concentration of STMP/STPP 2%’, however, such a value is not seen in a Fig. 1.
Lines 187-188: Is there any reference cited to this, as the authors received a relatively thick material?
Line 201: 30,09 % value does not appear in Fig. 2.
Lines 220, 224: Instead of ‘smaller than’ there should be ‘lower than’.
Line 269: Instead of ‘mechanical properties’ there should be ‘mechanical parameters’.
Figs 1-5: According to the requirement of Polish Journal of Food and Nutrition
PJFNS-00284-2019-01
Science, results should not be repeated, and the same concerns data in tables and figures: “Do not display the data in both tabular and graphic form”.
Section Editor recommendation
The authors are strongly invited to comply with the rebiewer’ suggestions
1
The Physical, Physicochemical, Mechanical and Sensory Properties of Bioplastics From Phosphate Acetylated Arenga Starches
Abdul Rahim1*, Safitri2, Syahraeni Kadir1, Muhardi1, Syamsuddin Laude1, Jusman3 and Steivie Karouw4
1Faculty of Agriculture, Tadulako University,
Jalan Soekarno Hatta Km.9 No.32 Palu, Central Sulawesi, 94118 Indonesia.
2Graduates Faculty of Agriculture, Tadulako University,
Jalan Soekarno Hatta Km. 9 No.32 Palu, Central Sulawesi, 94118 Indonesia
3Faculty of Mathematics and Natural Science, Tadulako University, Jalan Soekarno Hatta Km. 9 No.32 Palu, Central Sulawesi, 94118 Indonesia
4Indonesian Palm Crops Research Institute, Jalan Raya Mapanget PO BOX 1004 Manado Nort Sulawesi, Indonesia.
*Corresponding author, e-mail: [email protected] Telephone: +62451429738, Mobile number: +6285397897809
Abstract
Bioplastics are alternative to plastic packaging made from renewable natural materials.
They have been observed to have a great potential for wider application due to their environmental-friendliness and ease of degradation. This research therefore aimed to evaluate the physical, physicochemical, mechanical, and sensory characteristics of bioplastics made from native arenga starch (NAS) and phosphate acetylated arenga starches (PAAS). The PAAS was obtained from theby dual modification of NAS through acetylation using 5% acetic anhydride and crosslinking using a mixture of sodium trimetaphosphate (STMP) and sodium tripolyphosphate (STPP) at 99/:1 (w/w). The concentrations of the mixture were varied at 2, 4, 6, 8, 10, and 12% (w/w) of the starch. The thickness, water holding capacity (WHC), oil holding capacity (OHC), water vapor transmission rate (WVTR), water content, biodegradation, fourier transform infrared (FT-IR) spectroscopy, tensile strength, elongation at break, Young’s modulus and sensory properties of the NAS and PAAS bioplastics were investigated. The results showed
Formatted: Font: Italic Formatted: Font: Italic
the use of mixture concentrations of STMP/STPP in concentrations from 2 to 6% improved all the properties of the PAAS bioplastics while the thickness of the NAS and PAAS were generally uniform. The WHC of the NAS bioplastic was higher than PAAS. while Tthe OHC and WVTR of the PAAS bioplastic increased with the increment in the concentration of the STMP/STPP mixture. Furthermore, the water content of the PAAS bioplastics was lower than NAS while the weight loss due to biodegradation of the NAS was higher than the PAAS. Meanwhile, both NAS and PAAS can be decomposed completely in the soil. However, tThe PAAS bioplastics were characterized by FTIR and this confirmed the acetylation and crosslinking activities between the arenga starch molecules. Generally, tThe elongation at break, color, and texture of the PAAS bioplastics were higher than NAS bioplastic.
Keywords: NASnative arenga starch, acetylation, cross-linking, sodium trimetaphosphate, sodium tripolyphosphate PAAS, bioplasticfilmss, mixture concentrations of STMP/STPP
INTRODUCTION
Packaging is the final part of the processes involved in the production of food and non- food products purposely to increase shelf life, improve consumer acceptance, and as a means of providing support for the distribution and expansion of product marketing [Prasteen et al., 2018].
The major material used for this purpose is plastic and this has led to a continuous increase in its waste thereby causing environmental pollution because it is nonbiodegradable, its recycling process is quite expensive, and has the ability to contaminate foods [Ogunrinola & Akpan, 2018]. There is, however, the urgent need to find alternative materials for packaging and one of these is the bioplastics due to its safe and biodegradable nature.
Bioplastics are produced from renewable natural materials and have been observed to have the potentials of being an alternative to plastic packaging due to its environmental friendliness and easy degradation. Therefore, there is an urgent need for bioplastics due to the rapid increase in the pace of plastic production and air pollution causing several health risks because of their toxic nature [Jain & Tiwari, 2015]. Bioplastics are, however, very suitable alternatives to improve the quality of life and maintain a pollution-free planet [Keziah et al., 2018].
Commented [M1]: This is not true in the light of statistical analysis . There were no statistical differences between the samples for several parameters. Please, correct the sentence Commented [M2]: OHC of PAAS bioplastics did not differ statistically significantly (acc. information in text)
Commented [M3]: There were no statistical differences between the samples (acc. information in text)
Commented [M4]: “color and texture were higher” – unclear.
Formatted: Not Highlight
