Innovative Thermoplastic Starch Based Biodegradable Packaging For Food Industies Application.

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UNIVERSITI TEKNIKAL MALAYSIA MELAKA

INNOVATIVE THERMOPLASTIC STARCH BASED

BIODEGRADABLE PACKAGING FOR FOOD INDUSTRIES

APPLICATION

This report submitted in accordance with requirement of the Universiti Teknikal Malaysia Melaka (UTeM) for the Bachelor Degree of Manufacturing Engineering

(Engineering Materials)

by

MAZLIAH BINTI MAZLAN B050810283

FACULTY OF MANUFACTURING ENGINEERING 2011


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UNIVERSITI TEKNIKAL MALAYSIA MELAKA

BORANG PENGESAHAN STATUS LAPORAN PROJEK SARJANA MUDA

TAJUK: INNOVATIVE THERMOPLASTIC STARCH BASED BIODEGRADABLE PACKAGING FOR FOOD INDUSTRIES APPLICATION

SESI PENGAJIAN: 2010/ 11 Semest er 2

Saya MAZLIAH BINTI MAZLAN

mengaku membenarkan Laporan PSM ini disimpan di Perpust akaan Universit i Teknikal Malaysia Melaka (UTeM) dengan syarat -syarat kegunaan sepert i berikut : 1. Laporan PSM adalah hak milik Universit i Teknikal Malaysia Melaka dan penulis. 2. Perpust akaan Universit i Teknikal Malaysia Melaka dibenarkan membuat salinan

unt uk t uj uan pengaj ian sahaj a dengan izin penulis.

3. Perpust akaan dibenarkan membuat salinan laporan PSM ini sebagai bahan pert ukaran ant ara inst it usi pengaj ian t inggi.

4. **Sila t andakan (√)

SULIT

TERHAD

TIDAK TERHAD

(Mengandungi maklumat yang berdarj ah keselamat an at au kepent ingan Malaysia yang t ermakt ub di dalam AKTA RAHSIA RASMI 1972)

(Mengandungi maklumat TERHAD yang t elah dit ent ukan oleh organisasi/ badan di mana penyelidikan dij alankan)

Alamat Tet ap:

J7743, KM32 Jalan Salim, Kampung Bat u Gaj ah, 77300 Merlimau, Melaka.

Tarikh: _________________________

Disahkan oleh:

PENYELIA PSM

Tarikh: ______________________

** Jika Laporan PSM ini SULIT at au TERHAD, sila lampirkan surat daripada pihak berkuasa/ organisasi berkenaan dengan menyat akan sekali sebab dan t empoh laporan PSM ini perlu dikelaskan sebagai SULIT at au TERHAD.


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DECLARATION

I hereby, declared this report entitled “Innovative Thermoplastic Starch based Biodegradable Packaging for Food Industries Application” is the results of my

own research except as cited in references.

Signature : ………

Author’s Name : Mazliah binti Mazlan


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APPROVAL

This report is submitted to the Faculty of Manufacturing Engineering of UTeM as a partial fulfillment of the requirements for the Degree in Bachelor of Manufacturing Engineering (Engineering Materials). The member of the supervisory committee is as follow:

……… Supervisor


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ABSTRAK

Penyelidikan ini menunjukkan prestasi komposit plastik biolupus yang menggunakan tepung ubi kayu (TS) dan polypropylene (PP) sebagai bahan utama matriks dengan

penambahan serat gentian tebu (SCFC) sebagai penguat dan gliserol sebagai bahan tambah pemplastik. Tujuan utama penyelidikan ini adalah untuk membuat bungkusan plastik biolupus untuk industri makanan dengan menggunakan kaedah pencampur dalaman yang dinamakan sebagai PTSG Biodegradable Hybrid

Composite. Kesan penggunaan hampas tebu di dalam komposit ini dikaji dengan

lebih lanjut dan hasil komposit yang baik telah dicadangkan. Sampel komposit dihasilkan dengan menggunakan formula pencampuran yang berbeza dengan menggunakan kaedah campuran dan mampatan. Bagi mencapai objektif penyelidikan ini, pengujianan lanjutan untuk mengenalpasti sifat-sifat komposit tersebut dilakukan melalui ujian tegangan, ujian hentaman, dan ujian lenturan. Ujian-ujian ini dilakukan bagi menentukan sifat-sifat mekanikal bahan komposit tersebut. Kemudian, diikuti dengan penilaian sifat persekitaran PTSG Biodegradable Hybrid Composite seperti

ujian biolupus, uji penyerapan air dan ujian pembengkakan tebal. Dalam rangka untuk mengetahui morfologi patahan sampel, pemerhatian melalui mikroskop imbasan elektron (SEM) telah dijalankan. Peningkatan kadar tepung ubi telah meningkatkan kadar pelupusan, penyerapan air dan pembengkakan tebal yang dihasilkan oleh komposit. Perumusan yang terbaik adalah pada kombinasi 90% PP,

10% TS 1% SCFC dan 3% glycerol untuk PTSG Biodegradable Hybrid Composite

yang mempunyai potensi kinetik pelupusan sebanyak 0.014%/hari bagi penurunan berat yang memberikan cirri-ciri potensi dalam industri pembungkusan makanan. Secara keseluruhan, semua tujuan kajian yang dinyatakan telah tercapai dengan jayanya.


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ABSTRACT

This research shows the performance of biodegradable plastic composite using tapioca starch (TS) and polypropylene (PP) as a primary matrix material with addition of sugar cane fiber cellulose (SCFC) as reinforcement and glycerol as additive plasticizer. The main objective of this research is to fabricate a biodegradable plastic packaging for food industries using an internal mixer method which produced the novel biocomposites that simply named as PTSG Biodegradable Hybrid Composite. The effect of SCFC loading was studied as to establish the best formulation of the PTSG Biodegradable Hybrid Composite. The composites were fabricated into thin sheets using a hot compression molding machine. The PTSG Biodegradable Hybrid Composite were tested for tensile test, impact test, and flexural test. Then, the environmental properties were determined through soil burying test, weathering test, water absorption test and thickness swelling test. The fracture morphology of the samples was observed under scanning electron microscope (SEM). The increasing of tapioca starch content had significantly increased the degradation, water absorption and swelling thickness of produced composite. The optimum compounding formulation of the fabricated composites was observed at the combination of 90 wt.% of PP, 10 wt.% of TS, 1 wt.% of SCFC and 3 wt.% of glycerol for PTSG Biodegradable Hybrid Composites that have the potential kinetic of degradation at 0.014 %/day of weight reduction which could potentially applied in the real green food packaging industries as one of new candidates for future food packaging materials. In overall, all the listed research objectives were successfully achieved from this preliminary research


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ACKNOWLEDGEMENT

Bismillahirrahmanirrahim,

I am so thankful to Allah S.W.T for giving me patient and spirit throughout this project until the research is successfully completed. With the mercifulness from Allah therefore I can produce a lot of idea to this project.

I am indebted to my supervisor, Mr. Jeefferie bin. Abd Razak, lecturer from the Faculty of Manufacturing Engineering for his advice, insightful comments and support. Thank for your guide and without your guide this research will not be completed and well organized. Not forgetting for my panels, Dr. Noraiham binti Mohamad and Miss Siti Rahmah binti Shamsuri for the continuous support and constructive ideas. Thank you very much.


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DEDICATION

Emak, Abah and All My Family Members

Along, Angah, Kak De, Kak Nak, Atam, Atih, Achik, Mamat, Ida My Bear

My Lecturer, Che Jep Lovely Friends 4 BMFB 2011


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TABLE OF CONTENT

Abstrak i

Abstract ii

Acknowledgement iii

Dedication iv

Table of Content v

List of Tables vi

List of Figures vii

List of Abbreviations viii

1. INTRODUCTION 1

1.1 Introduction 1

1.2 Objectives 3

1.3 Problem Statement 3

1.4 Significant of Study 4

1.5 Thesis Overview 4

2. LITERATURE REVIEW 5

2.1 Introduction 5

2.2 Composite 5

2.3 Polymer Matrix Composites (PMC) 6

2.4 Polypropylene (PP) as Matrix Materials 8

2.5 Reinforcement 9

2.6 Natural Fiber 11

2.7 Sugar Cane Fiber Cellulose (SCFC) as Natural Fiber 12 2.7.1 Properties of Sugar Cane Fiber Cellulose (SCFC) 14

2.7.1.1 Physical Properties 14

2.7.1.2 Mechanical Properties 14


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2.9 Tapioca Starch as Matrix 16

2.10 Glycerol as Plasticizer 18

2.10.1 General Properties of Glycerol 19

2.10.2 Physical Properties of Glycerol 19

2.11 Mechanical Properties of the Composites 20

2.11.1 Tensile Properties 20

2.11.2 Impact Properties 21

2.11 3 Flexural Properties 22

2.12 Environmental Properties Evaluation for PTSG Biodegradable

Hybrid Composite 23

2.12.1 Biodegradation Test 23

2.12.2 Water Absorption Test 25

2.12.3 Thickness Swelling Test 27

2.13 Morphology Observation 27

3. METHODOLOGY 30

3.1 Introduction 30

3.2 Methodology 30

3.2.1 Flow Chart of Methodology 31

3.3 Materials 31

3.3.1 Tapioca Starch (TS) 33

3.3.2 Sugar Cane Fiber Cellulose (SCFC) 34

3.3.3 Glycerol 34

3.3.4 Polypropylene 35

3.4 Raw Materials Preparation 36

3.4.1 Sugar Cane Fiber Cellulose (SCFC) Drying Process 36

3.4.2 Crushing Process 37

3.5 Characterization of Sugar Cane Fiber Cellulose 38

3.5.1 Drying Profile Study 38

3.5.2 Density Measurement 38

3.5.3 Morphological Observation 39

3.6 Sample Fabrication 40


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3.6.2 Hot Compression Molding 42

3.7 Mechanical Testing 42

3.7.1 Tensile Test 43

3.7.2 Impact Test 44

3.7.3 Flexural Test 44

3.8 Environmental Properties Evaluation for PTSG Biodegradable

Hybrid Composite 46

3.8.1a Weathering Test 46

3.8.1b Soil Test 46

3.8.2 Water Absorption Test 47

3.8.3 Thickness Swelling Test 47

4. RESULTS AND DISCUSSIONS 48

4.1 Introduction 48

4.2 Raw Material Characterization 48

4.2.1 SCFC Density Measurement 48

4.3 The Study on the processability of PTSG Biodegradable Hybrid

Composite 51

4.3.1 Processing characteristics of PTSG Biodegradable Hybrid

Composite 51

4.3.2 Torque analysis of PTSG Biodegradable Hybrid Composite 51 4.4 Characterization of Mechanical properties for PTSG Biodegradable

Hybrid Composite 53

4.4.1 Tensile Test Analysis for PTSG Biodegradable Hybrid

Composite 53

4.4.2 Flexural Test / Three Point Bending Analysis for PTSG

Biodegradable Hybrid Composite 57

4.4.3 Charpy Impact Strength Analysis for PTSG Biodegradable Hybrid

Composite 59

4.5 Characterization of environmental evolution for PTSG Biodegradable

Hybrid Composite 61

4.5.1 Weathering properties of PTSG Biodegradable Hybrid


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4.5.2 Soil Properties of PTSG Biodegradable Hybrid Composite 65 4.6 Characterization of water absorption properties for PTSG Biodegradable

Hybrid Composite 69

4.7 Characterization of thickness swelling properties for PTSG Biodegradable

Hybrid Composite 70

4.8 SEM analysis of tensile test fractured surface of PTSG Biodegradable

Hybrid Composite 72

5. CONCLUSION AND RECOMMENDATIONS 75

5.1 Conclusion 75

5.2 Recommendations 77

REFERENCES 78

APPENDICES

A Gantt chart for PSM I I

B American Standard Testing Material (2000) Standard Test Method for Tensile Properties of Plastics

C American Standard Testing Material (2000) Standard Test Methods for Flexural Properties of Unreinforced and Reinforced Plastics and Electrical Insulating Materials E Results of Hardness Test

D American Standard Testing Material (2000) Standard Test Methods for Determining the Izod Pendulum Impact Resistance of Plastics

E American Standard Testing Material (2000) Standard Test Methods for Water Absorption of Plastics


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LIST OF TABLES

2.1 Melting and glass transition temperature for selected polymers 9

2.2 Bagasse chemical compositions 13

2.3 Physical characteristic for some common types of fiber 14

2.4 Mechanical properties of some natural fibers 15

2.5 Physical properties of TS/PCL blends using granular (TS) starch in

various proportions 17

2.6 Specifications for tapioca starch by Thai Tapioca Flour Industry

Trade Association 17

2.7 General information of glycerol 19

2.8 Physical properties of glycerol 19

3.1 Standard Specification of native cassava starch for modification purpose 33 3.2 The basic physical properties of the glycerol used 35

3.3 The Polypropylene (PP) Typical Properties 36

3.4 The PTSG Biodegradable Hybrid Composites formulation 40 3.5 PTSG Biodegradable Hybrid Composite formulation 41 4.1 Density measurement of sugar cane fiber cellulose 49 4.2 Density measurement of some natural fibers and raw material 50

4.3 Mechanical properties of some natural fibers 51

4.4 Impact properties of PTSG Biodegradable Hybrid Composite 60 4.5 Before and after observation of weathering test 63 4.6 Weight before and after weathering test; Percentages of

weight reduction (%). 65

4.7 Before and after observation of soil burial test 66 4.8 Weight before and after burying test; Percentages of


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LIST OF FIGURES

2.1 Polymerization of propylene to polypropylene 8

2.2 Fiber arrangement patterns in the layer of fiber reinforce composite

Material 10

2.3 Classification of natural fibers 12

2.4 Part of the sugar cane 12

2.5 Tensile strength and %strain of LDPE composite sheets 21 2.6 Tensile strengths of LDPE, LDPE/S and LDPE/MS blends 24 2.7 Percentage water absorption of starch-filled poly

(styrene-co-butyl acrylate) polyester nonwoven composites

at room temperature for 24 hrs and 8 days 26

2.8 Rate of water absorption of starch-filled

poly (styrene-co-butyl acrylate) polyester nonwoven composites

at room temperature 26

2.9 Percentage thickness swelling of starch-filled

poly (styrene-co-butyl acrylate) polyester nonwoven composites

at room temperature 27

2.10 SEM micrographs of the cryogenically fractured surface of (a) and (b) 80/20 LLDPE/TS blend

(c) 80/20/2 LLDPE/S/S-g-OSA (DS = 0.024) blend, and

(d) 80/20/2 LLDPE/S/S-g-OSA (DS = 0.045) blend 28 2.11 SEM micrographs of kenaf fiber surface in composites

(A) 100μm (at 200x) and (B) 10μm (at 500x) 29

3.1 Flow chart of methodology 32

3.2 Tapioca starch 33

3.3. Sugar cane fiber cellulose 34

3.4 Glycerol 35


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3.6 Drying sugar cane fiber cellulose in the oven model

UFB 400, MEMMERT 37

3.7 Rotor mill machine 37

3.8 Drying SCFC in the laboratory oven 38

3.9 Electronic Densimeter 39

3.10 SEM model EVO 50 44

3.11 HAAKE Rheomix OS 41

3.12 Hot compression molding 42

3.13 Universal Testing Machine (UTM) 43

3.14 Tensile specimen 43

3.15 Charpy Types Specimen 44

3.16 Flexural testing at three-point bending set-up 45 3.17 Standard test configuration of flexural test 45 4.1 Average plot of torque value (Nm) versus time (minutes) for the

PTSG Biodegradable Hybrid Composite with different

wt.% of filler loading 51

4.2 Tensile strength of PTSG Biodegradable Hybrid composite

at different composition of PP/TS/SCFC/glycerol 54 4.3 Percentage of Elongation for PTSG Biodegradable Hybrid composite

at different composition of PP/TS/SCFC/glycerol 56 4.4 Tensile Modulus of PTSG Biodegradable Hybrid composite

at different composition of PP/TS/SCFC/glycerol 56 4.5 Flexural Strength of PTSG Biodegradable Hybrid Composite

at different composition of PP/TS/SCFC/glycerol 58 4.6 Flexural Modulus of PTSG Biodegradable Hybrid Composite

at different composition of PP/TS/SCFC/glycerol 58 4.7 Impact strength of PTSG Biodegradable Hybrid composite

at different composition of PP/TS/SCFC/glycerol 61 4.8 Comparison of normal, weathering and soil burial degradation test


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4.9 Water absorption characteristic PTSG Biodegr adable Hybrid Composite at different composition of PP/TS/SCFC/glycerol

within 10 days of immersion. 70

4.10 Comparison of thickness deflection PTSG Biodegradable Hybrid Composite at different composition of PP/TS/SCFC/glycerol

within 10 days 72

4.11 SEM micrograph showed the fractured surface of the virgin pp sample at a) 500X and

b) 1 000X of magnification 73

4.12 SEM micrograph showed the fractured surface of the PTSG Biodegradable Hybrid Composite with various compositions of PP/TS/SCFC/glycerol

a) 100/0/1/3 b) 90/10/1/3 c) 80/20/1/3 d) 70/30/1/3 and


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LIST OF ABBREVIATIONS

ASTM American Standard Testing of Materials CMC Ceramic Matrix Composite

DS Degrees of Substitution

DSC Differential Scanning Calorimetry

Eg. Example

et al. and others etc. Et cetera

LDPE Low Density Polyethylene

LLDPE Linear Low Density Polyethylene

MAPP Maleic-Anhydride Grafted Polypropylene MMC Metal Matrix Composite

MS Modified starch

PC Polycarbonates

PCL Polycaprolactrone PHA Polyhydroxyalkanoate

PHBV polyhydroxybutyrate and hydroxyvalerate PLA polylactic acid

PMC Polymer Matrix Composite

PP Polypropylene

TS / SCFC Tapioca starch reinforced sugar cane fiber cellulose

S Starch

SCFC Sugar Cane Fiber Cellulose SEM Scanning electron microscopy S-g-OSA Succinylated Starches

TGA Thermo Gravimetric Analyzer

TS Tapioca Starch

Wt% Percent of weight fraction WA Water Absorption


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CHAPTER 1

INTRODUCTION

1.1 Introduction

A plastic material is one of a wide range of synthetic or semi-synthetic organic amorphous solid used in the manufacture of industrial products. Due to their versatility, plastic is great for packaging of a variety products such as processed and convenience foods, pharmaceuticals and medicines, cosmetics and toiletries, household and agricultural chemicals, petroleum product and detergent. Nowdays, plastic containers are successfully replacing glass, tin, metal, aluminum and paper containers in many applications. This is because plastics are typically polymers of high molecular mass, and may contain other substances to improve performance of the fabricated products. Therefore, the advantages of plastics are light and less bulky than other packaging materials that could be processed into any desired shape or form such as films, sheets and pouches. On the other hand, it saves costs of storage and transportation because of lower volume, easy coloring, no rusting and first-rate water resistance. Although plastic package have great advantages, however they also have some limitations that includes some chemical attack on particular plastics, tendency to creep, less heat resistance, lower gas barrier and lower dimensional stability (Athalye, 2002).

Into the bargain, there are grave problems connected with the analytical control of such materials which are toxic hazards from the modified plastics and also from their degradation products, increased costs and the possible encouragement of litter. In order to trim down this problem, the application of biodegradable material as an alternative choice is increasingly applied. Biodegradable which are often produced


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from renewable sources, are being increasingly sought after by food processors as part of a solution to environmental concerns over waste and the use of fossil fuels. The process is called biodegradation (Dong et al. 2008). Biodegradation is a natural

process by which organic chemicals in the environment are converted to simpler compounds, mineralized, and redistributed through the elemental cycles such as the carbon, nitrogen, and sulphur by the action of microorganism.

In this research, biodegradable polymer matrix composites (PMCs) were developed. There are two natural components were combined which are tapioca starch (TS) as a natural matrix material and sugar cane fiber cellulose (SCFC) as a natural biofiber. Sugar cane has good performance as filler reinforcement, together with the advantages to the environment when it combines with the tapioca starch matrix. Polypropylene (PP) and glycerol are being utilized as part of two mixtures as to produce the innovative formulation as well as to facilitate the processing. It is expected that the development of this product, will contribute to the world as novel biodegradable, non-toxic and non-allergenic bio environmental friendly natural green products.

There is considerable interest and noble aims in this research where to produce an alternative material by compounding tapioca starch (TS), polypropylene (PP), sugar cane fiber cellulose (SCFC) and glycerol to replace the existing non biodegradable plastic material in the commercial market. Thus, overall of this research is to formulate the biodegradable based composites filled with an agro-waste biofiller by using the internal mixer method in order to investigate and understand the behavior and properties as well as characteristic of the tapioca starch (TS), polypropylene (PP), sugar cane fiber cellulose (SCFC) and glycerol biocomposites or in short is namely as PTSG Biodegradable Hybrid Composite. Utilization of biodegradable based product will significantly reduce the need for synthetic polymer production at low cost, thereby producing a positive effect both environmentally and economically.


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1.2 Objective

The purposes of this study are:

• To formulate biodegradable packaging material for food industries by using internal mixer method combining the tapioca starch (TS), polypropylene (PP), sugar cane fiber cellulose (SCFC) and glycerol, in their formulations. • To establish and understand the mechanical, morphological and degradation

behavior of novel biocomposites containing tapioca starch (TS), polypropylene (PP), and sugar cane fiber cellulose (SCFC) and glycerol mixtures, in comparisons to other biocomposites.

1.3 Problem Statement

There are problems connected with the utilization of hydrocarbon plastic based materials which are toxic hazards from the modified plastics and also from their degradation products, high costs and possible encouragement of litter. Allocated to this problem, it is important to produce innovative products which combine the utilization of natural filler with other elements such as glass, plastics and synthetics material. Ecological concerns have resulted in overwhelming interest in natural and compostable materials and issues related with the biodegrability and environmental safely that are becoming corresponding important (Yu et al., 2007). Biodegradable or

environmentally acceptable materials have attained increasing interest in few decades to the researchers and manufactures due to environmental pressure derived from the consumption of petroleum based materials, difficulties in degradation in a landfill and composting environments (Liu et al. 2006; Huda et al. 2007). Starch is one of

the most promising materials for biodegradable plastics because of its versatile biopolymer characteristic with immense potential and low price for application in the food industries (Mohanty et al., 2000). However, starch was mostly water soluble,

difficult to process and brittle in nature when it is used without the addition of plasticizer. Furthermore, the mechanical properties are very sensitive to moisture


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content, which is difficult to control and predict. In principle, some properties of starch could be significantly improved by blending it with polymer (Dufresne et al.,

2000). As a result, the TS, PP, SCFC and glycerol are combined as to formulate the new potential biodegradable packaging material for food industries application.

1.4 Significant of Study

In this research, the noble aim is to develop the PTSG Biodegradable Hybrid Composite for the food packaging application. As a consequence, by conducting this research, it is expected that it will be benefited to the environment that suffer with non-degradable waste of plastic food packaging caused by uncontrolled solid waste disposal and extensive utilization of this necessity. Development of this novel food packaging alternative will create potential solution to the environmental friendly and safe packaging medium either for food, consumer or environment as a whole.

1.5 Thesis Overview

This thesis is divided into five chapters that describe the analytical and experimental research performed. The First Chapter is an introduction to the study that brief about objectives, problem statement, significant of study and the thesis overview. Chapter Two present the literature review that relates to the theories on composites and previous investigations on the biocomposites. The important element that included in this chapter is about the types of properties for SCFC and TS and also related experimental testing. Chapter Three, provides details explanations on the methodology used for overall research work, raw materials, procedure property analysis that had been done. In Chapter Four, the result of the characterization and measurement of various engineering properties for the fabricated biocomposites were explained in details. The final chapter (Chapter 5) concludes the overall results obtained from this research. In this chapter, it explains either the objectives of this study are achieved or not. The recommendation for future project also has been included in this Chapter 5.


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CHAPTER 2

LITERATURE REVIEW

2.1 Introduction

This chapter review related studies done by previous researcher on the tapioca starch (TS) as matrix whiles the sugar cane fiber cellulose (SCFC) as reinforcement in the biocomposites product based development. Through this chapter, the study on the SCFC, TS and Polypropylene (PP) engineering properties had been highlighted and extensively reviewed. The literature review mainly focused on the various types of engineering properties and related experimental testing will be studied and discussed. The fundamental of composites were reviewed in the first following section and followed by the engineering properties from the existing research of the biocomposites, as well as the degradation of the composites.

2.2 Composites

A composite material is a material system that composed of a suitably arranged mixture or combination of two or more micro or macroconstituents with an interface separating them that differ in form and chemical composition and are essentially insoluble in each other (Smith et al. 2000). An engineering importance of a

composite material is that two or more distinctly different materials combine to form a composite material that possesses properties that are superior, or important in some other manner, to the properties of the individual components (Smith et al. 2000).


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Thus, composites are those materials formed by aligning extremely strong and stiff constituents such as fibers and particulates in a binder called matrix. The materials in this category have excellent mechanical properties. There are two components in the composite, which are reinforcing phase and matrix phase. Polymers, ceramic and metals have found their application as matrix materials. The reinforcing phase is other component and is called reinforcement and could be fiber, particulate or laminar (Gupta, 2005). According to Matthews and Rawlings (2002), each of materials (i.e., matrix and reinforcement) must exist of more than 5 wt% to be classified as composites material. The purposed of introducing the composites material is to improve the properties that have been performed by monolithic material. Thus, the composite is expected to improve the mechanical characteristics such as stiffness, toughness, ambient and high-temperature resistance (Callister, 2003).

According to Callister (2003), the composites materials are classified by the geometry of reinforcement and the types of matrix materials used in its constituent. As a result, there are three main types of geometries of the reinforcement which are particle-reinforced, fiber-reinforced and structural composites (Callister, 2003). Types of matrix used in composites also can be divided into four types, namely as polymer-matrix composite (PMC), metal-matrix composites (MMC), ceramics-matrix composites (CMC), and carbon-carbon composites (CCC) (Matthews and Rawlings, 2002; Callister, 2003; Taj et al. 2007). In this study, PMC becomes as the

topic of investigation.

2.3 Polymer Matrix Composites (PMC)

As the terms implied, the polymer matrix composites consists of polymeric material as the matrix material and fiber as the reinforcement elements (Luz et al. 2007).

Research and engineering interest has been shifted from the monolithic material to fiber-reinforced polymeric material (Wambua et al. 2003). Polymer matrix


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enormous applications of PMC have exhibited various performances that cannot be performed by any monolithic material (Wambua et al. 2003).

There are three types of major classes in polymeric materials which are thermoplastics, thermosets, and elastomers (Kalpakjian, 2006). Reinforcement of polymers by strong fibrous network permits fabrication of PMC characterized by the properties such as high tensile strength, high stiffness, high fracture toughness, good abrasion resistance, good corrosion and puncture resistance but the main disadvantages are low thermal resistance and high coefficient of thermal expansion (Liu et al. 2007; Taj et al. 2007).

The extensive used of PMC as daily life components, exhibits that the PMC has low density, ρ where the benefit of low density becomes apparent when the tensile modulus per unit mass, E/ρ (specific modulus), and tensile strength per unit mass, σ/ρ (specific strength), are considered. Contrarily, it is also observed that the used of PMC has resulted in the reduction of flexural and tensile strength of the fabricated composites (Wambua et al. 2003).

There were limitations of PMC which need to be considered, such as their low maximum working temperatures, high coefficient of thermal expansion, dimensional instability, and sensitivity to radiation and moisture (Hanlon et al. 1998; Selke et al.

2004; Harper, 2006). This leads to a degree of environmental degradation greater than that experienced by the component of material alone. Until early 1970s, the focus was given on the preventing the plastic degradation to avoid the loss in the performance of the plastic properties. The extent of degradation was generally measured by the loss percentages of the useful properties. It was stated that 90 percent loss in the tensile strength was equivalent to total degradation, as this was sufficient to render the plastic object unusable. In the middle of 1980s, when concerns about solid waste disposal were increased, the interest in biodegradation intensified as some perceived it as a solution to the landfill crisis (Hanlon et al. 1998;


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from renewable sources, are being increasingly sought after by food processors as part of a solution to environmental concerns over waste and the use of fossil fuels. The process is called biodegradation (Dong et al. 2008). Biodegradation is a natural process by which organic chemicals in the environment are converted to simpler compounds, mineralized, and redistributed through the elemental cycles such as the carbon, nitrogen, and sulphur by the action of microorganism.

In this research, biodegradable polymer matrix composites (PMCs) were developed. There are two natural components were combined which are tapioca starch (TS) as a natural matrix material and sugar cane fiber cellulose (SCFC) as a natural biofiber. Sugar cane has good performance as filler reinforcement, together with the advantages to the environment when it combines with the tapioca starch matrix. Polypropylene (PP) and glycerol are being utilized as part of two mixtures as to produce the innovative formulation as well as to facilitate the processing. It is expected that the development of this product, will contribute to the world as novel biodegradable, non-toxic and non-allergenic bio environmental friendly natural green products.

There is considerable interest and noble aims in this research where to produce an alternative material by compounding tapioca starch (TS), polypropylene (PP), sugar cane fiber cellulose (SCFC) and glycerol to replace the existing non biodegradable plastic material in the commercial market. Thus, overall of this research is to formulate the biodegradable based composites filled with an agro-waste biofiller by using the internal mixer method in order to investigate and understand the behavior and properties as well as characteristic of the tapioca starch (TS), polypropylene (PP), sugar cane fiber cellulose (SCFC) and glycerol biocomposites or in short is namely as PTSG Biodegradable Hybrid Composite. Utilization of biodegradable based product will significantly reduce the need for synthetic polymer production at low cost, thereby producing a positive effect both environmentally and economically.


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1.2 Objective

The purposes of this study are:

• To formulate biodegradable packaging material for food industries by using internal mixer method combining the tapioca starch (TS), polypropylene (PP), sugar cane fiber cellulose (SCFC) and glycerol, in their formulations.

• To establish and understand the mechanical, morphological and degradation behavior of novel biocomposites containing tapioca starch (TS), polypropylene (PP), and sugar cane fiber cellulose (SCFC) and glycerol mixtures, in comparisons to other biocomposites.

1.3 Problem Statement

There are problems connected with the utilization of hydrocarbon plastic based materials which are toxic hazards from the modified plastics and also from their degradation products, high costs and possible encouragement of litter. Allocated to this problem, it is important to produce innovative products which combine the utilization of natural filler with other elements such as glass, plastics and synthetics material. Ecological concerns have resulted in overwhelming interest in natural and compostable materials and issues related with the biodegrability and environmental safely that are becoming corresponding important (Yu et al., 2007). Biodegradable or environmentally acceptable materials have attained increasing interest in few decades to the researchers and manufactures due to environmental pressure derived from the consumption of petroleum based materials, difficulties in degradation in a landfill and composting environments (Liu et al. 2006; Huda et al. 2007). Starch is one of the most promising materials for biodegradable plastics because of its versatile biopolymer characteristic with immense potential and low price for application in the food industries (Mohanty et al., 2000). However, starch was mostly water soluble, difficult to process and brittle in nature when it is used without the addition of plasticizer. Furthermore, the mechanical properties are very sensitive to moisture


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content, which is difficult to control and predict. In principle, some properties of starch could be significantly improved by blending it with polymer (Dufresne et al., 2000). As a result, the TS, PP, SCFC and glycerol are combined as to formulate the new potential biodegradable packaging material for food industries application.

1.4 Significant of Study

In this research, the noble aim is to develop the PTSG Biodegradable Hybrid Composite for the food packaging application. As a consequence, by conducting this research, it is expected that it will be benefited to the environment that suffer with non-degradable waste of plastic food packaging caused by uncontrolled solid waste disposal and extensive utilization of this necessity. Development of this novel food packaging alternative will create potential solution to the environmental friendly and safe packaging medium either for food, consumer or environment as a whole.

1.5 Thesis Overview

This thesis is divided into five chapters that describe the analytical and experimental research performed. The First Chapter is an introduction to the study that brief about objectives, problem statement, significant of study and the thesis overview. Chapter Two present the literature review that relates to the theories on composites and previous investigations on the biocomposites. The important element that included in this chapter is about the types of properties for SCFC and TS and also related experimental testing. Chapter Three, provides details explanations on the methodology used for overall research work, raw materials, procedure property analysis that had been done. In Chapter Four, the result of the characterization and measurement of various engineering properties for the fabricated biocomposites were explained in details. The final chapter (Chapter 5) concludes the overall results obtained from this research. In this chapter, it explains either the objectives of this study are achieved or not. The recommendation for future project also has been included in this Chapter 5.


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CHAPTER 2

LITERATURE REVIEW

2.1 Introduction

This chapter review related studies done by previous researcher on the tapioca starch (TS) as matrix whiles the sugar cane fiber cellulose (SCFC) as reinforcement in the biocomposites product based development. Through this chapter, the study on the SCFC, TS and Polypropylene (PP) engineering properties had been highlighted and extensively reviewed. The literature review mainly focused on the various types of engineering properties and related experimental testing will be studied and discussed. The fundamental of composites were reviewed in the first following section and followed by the engineering properties from the existing research of the biocomposites, as well as the degradation of the composites.

2.2 Composites

A composite material is a material system that composed of a suitably arranged mixture or combination of two or more micro or macroconstituents with an interface separating them that differ in form and chemical composition and are essentially insoluble in each other (Smith et al. 2000). An engineering importance of a composite material is that two or more distinctly different materials combine to form a composite material that possesses properties that are superior, or important in some other manner, to the properties of the individual components (Smith et al. 2000).


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Thus, composites are those materials formed by aligning extremely strong and stiff constituents such as fibers and particulates in a binder called matrix. The materials in this category have excellent mechanical properties. There are two components in the composite, which are reinforcing phase and matrix phase. Polymers, ceramic and metals have found their application as matrix materials. The reinforcing phase is other component and is called reinforcement and could be fiber, particulate or laminar (Gupta, 2005). According to Matthews and Rawlings (2002), each of materials (i.e., matrix and reinforcement) must exist of more than 5 wt% to be classified as composites material. The purposed of introducing the composites material is to improve the properties that have been performed by monolithic material. Thus, the composite is expected to improve the mechanical characteristics such as stiffness, toughness, ambient and high-temperature resistance (Callister, 2003).

According to Callister (2003), the composites materials are classified by the geometry of reinforcement and the types of matrix materials used in its constituent. As a result, there are three main types of geometries of the reinforcement which are particle-reinforced, fiber-reinforced and structural composites (Callister, 2003). Types of matrix used in composites also can be divided into four types, namely as polymer-matrix composite (PMC), metal-matrix composites (MMC), ceramics-matrix composites (CMC), and carbon-carbon composites (CCC) (Matthews and Rawlings, 2002; Callister, 2003; Taj et al. 2007). In this study, PMC becomes as the topic of investigation.

2.3 Polymer Matrix Composites (PMC)

As the terms implied, the polymer matrix composites consists of polymeric material as the matrix material and fiber as the reinforcement elements (Luz et al. 2007). Research and engineering interest has been shifted from the monolithic material to fiber-reinforced polymeric material (Wambua et al. 2003). Polymer matrix composite is the common types of matrix composites used for a few decades. The


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enormous applications of PMC have exhibited various performances that cannot be performed by any monolithic material (Wambua et al. 2003).

There are three types of major classes in polymeric materials which are thermoplastics, thermosets, and elastomers (Kalpakjian, 2006). Reinforcement of polymers by strong fibrous network permits fabrication of PMC characterized by the properties such as high tensile strength, high stiffness, high fracture toughness, good abrasion resistance, good corrosion and puncture resistance but the main disadvantages are low thermal resistance and high coefficient of thermal expansion (Liu et al. 2007; Taj et al. 2007).

The extensive used of PMC as daily life components, exhibits that the PMC has low density, ρ where the benefit of low density becomes apparent when the tensile modulus per unit mass, E/ρ (specific modulus), and tensile strength per unit mass, σ/ρ (specific strength), are considered. Contrarily, it is also observed that the used of PMC has resulted in the reduction of flexural and tensile strength of the fabricated composites (Wambua et al. 2003).

There were limitations of PMC which need to be considered, such as their low maximum working temperatures, high coefficient of thermal expansion, dimensional instability, and sensitivity to radiation and moisture (Hanlon et al. 1998; Selke et al. 2004; Harper, 2006). This leads to a degree of environmental degradation greater than that experienced by the component of material alone. Until early 1970s, the focus was given on the preventing the plastic degradation to avoid the loss in the performance of the plastic properties. The extent of degradation was generally measured by the loss percentages of the useful properties. It was stated that 90 percent loss in the tensile strength was equivalent to total degradation, as this was sufficient to render the plastic object unusable. In the middle of 1980s, when concerns about solid waste disposal were increased, the interest in biodegradation intensified as some perceived it as a solution to the landfill crisis (Hanlon et al. 1998; Selke et al. 2004; Harper, 2006).