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UNIVERSITI TEKNIKAL MALAYSIA MELAKA Faculty of Manufacturing Engineering THE EFFECTS OF GLASS WASTE AND GROG ON PHYSICAL AND MECHANICAL PROPERTIES IN PORCELAIN BY POWDER PRESSING METHOD Abu Bakar bin Aramjat Master of Manufacturing Engineering (Industrial Engineering) 2014 © Universiti Teknikal Malaysia Melaka

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UNIVERSITI TEKNIKAL MALAYSIA MELAKA

Faculty of Manufacturing Engineering

THE EFFECTS OF GLASS WASTE AND GROG ON PHYSICAL AND

MECHANICAL PROPERTIES IN PORCELAIN BY POWDER PRESSING

METHOD

Abu Bakar bin Aramjat

Master of Manufacturing Engineering (Industrial Engineering)

2014

© Universiti Teknikal Malaysia Melaka

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THE EFFECTS OF GLASS WASTE AND GROG ON PHYSICAL AND MECHANICAL PROPERTIES IN PORCELAIN BY POWDER PRESSING

METHOD

ABU BAKAR BIN ARAMJAT

A thesis submitted

in fulfillment of the requirements for the degree of Master of Manufacturing

Engineering (Industrial Engineering)

Faculty of Manufacturing Engineering

UNIVERSITI TEKNIKAL MALAYSIA MELA.KA

2014

© Universiti Teknikal Malaysia Melaka

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DECLARATION

I declare that this thesis entitled "The Effects of Glass Waste and Grog On Physical and

Mechanical Properties in Porcelain By Powder Pressing Method" is the result of my own

research except as cited in the references. The thesis has not been accept for any degree

and is not concurrently submitted in candidature of any other degree.

Signature ······~······· Name Abu Bakar bin Aramjat

Date 1 ith August 2014

© Universiti Teknikal Malaysia Melaka

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APPROVAL

I hereby declare that I have read this thesis and in my opinion this thesis is sufficient in

terms of scope and quality for the award of Master of Manufacturing Engineering

(Industrial Engineering).

Signature

Supervisor Name

Date

:.~ .... : Dr. Muhammad Zaimi bin Zainal Abidin

!~o~/uzc;

II. IUllAIMI Ulll 111 UIHl AltDU~ S...-Ledww

Feculty of Manufectllrinw Eftliftfffing Unlverslti Tebikel Mefey1la Melaka

Hang Tuah Jaye 76100 Durian Tung .. I, .,_Ile

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DEDICATION

This thesis is dedicated to my beloved wife Norhaslinda binti Md Nor and my sons

(Muhammad Akief Azfar, Muhammad Hadif Hafiy and Muhammad Hafidh Shafiy) . They

have been a source of motivation and strength during moments of despair and

discouragement, support has been shown in incredible ways recently.

© Universiti Teknikal Malaysia Melaka

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ABSTRACT

This research aims to study and investigate the effects of glass waste and grog on physical and mechanical properties in porcelain by using pressing method. Soda lime silicate glass is used as fluxing agent and fir_ed ceramic (grog) act as filler in por_c_elain body fabrication. Firstly, the recycle glass waste (glass window) and fired glazed tiles were crushed by using disc crusher until they passed through a sieve of less than 53µm. The glass powder and -gr0g was -thae-m:i;irnd wi th -based porceJai-n-bedy {5-0% kao-1-in, 25% fekl-sapr and 25% si-l-ica) with different percentage (5%glass-20% grog, 10%glass-15% grog, 15%glass-10% grog and 20%g]ass-5% grog). Then, green ceramic article is formed using uniaxial dry pressing method. All waste materials were analysed on their thermal behavior, chemical composition and mineralogical phase. In this study, the sintering temperature are varied at l 150°C, 1200°C, 1250°C, and 1280°C. Tue microstructure and phase present in sinterd products is analyzed using optic microscope, scanning electron microscope (SEM) and x­ray diffraction (XRD).The physical properties are determined using apparent porosity, bulk densi!Y and water absorption test. Mechanical analysis is carried out usin_g modulus of rupture to determine its mechanical properties. Tue results shown that the sintering temperature of porcelain decrease with the decreasing in percentage glass waste in cnmpQsition. Hence, it will decrease the water absorption and porosity of the porcelain. The physical-mechanical properties of porcelain will be affected by the sintering temperature, where physical-mechanical properties will be decreasing when the temperature reach at the optimum value (l 200°C). The best formulation composition is G5T20 (5% glass waste and 20% grog) and the optimum firing at 1200°C. Through the study, the enhancement of fabricated porcelain could be applied to the structural (such as floor and wall tile) applications through the advantage of mechanical and physical properties by high performance of strength, low water absorption, low porosity and high bulk density.

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ABSTRAK

Kajian ini bertujuan untuk mengkaji dan menganalisis kesan campuran sisa kaca dan 'sisa jasad bakar ubin ke atas sifat-sifat fizikal dan mekanikal di dalam jasad porse/in dengan menggunakan kaedah penekanan serbuk. Kaea soda-kapur-silikat digunakan sebagai fluk dan sisa jasad bakar ubin bertindak sebagai pengisi dalam fabrikasi jasad porselin. Sebagai permulaan, sisa kaca (kaca tingkap) dan jasad bakar ubin dihancurkan dengan menggunakan pengisar dan ditapis mengunakan penapis 1 OOµm. Serbuk sisa kaca dan sisa jasad bakar ubin dicampurkan di da/am formulasi jasad porselin (porselin tradisiona/ sebagai jasad piawaian) dengan peratusan yang berbeza (5%kaca-20% sisa ubin,, 10".kkaca-15%sisa ubin, 15%kaca-15%sisa ubin dan 20%kaca-5%sisa ubin). Kemudian, jasad anum dibentuk dengan menggunakan kaedah penekanan serbuk. Semua bahan sisa iaitu sisa kaca dan sisa jasad bakar ubin diana/isis ke atas sifat terma, komposisi kimia dan fasa minera/ogi. Da/am kajian ini, suhu pensinteran diubah pada 115Cf C, 120Cf C, 125CfC dan 128CfC. Mikrostruktur dan fasa dalam produk bakar dianalisis menggunakan mikroskop optik , mikroskop elektron imbasan (SEM) dan pembelauan sinar-X (XRD). Sifat fizikal ditentukan berdasarkan keliangan, ketumpatan dan ujian penyerapan air. Manakala, analisis mekanikal dijalankan menggunakan modulus kepatahan untuk menentukan kekuatan sampel. Keputusan di dalam kajian ini menunjukkan bahawa suhu pensinteran porselin berkurangan dengan peningkatan peratusan sisa kaca di dalam komposisi jasad porselin. Oleh itu, ia akan mengurangkan penyerapan air dan keliangan porselin. Sifat fizika/ mekanika/ porselin dipengaruhi o/eh suhu pensinteran, di mana sifat-sifat fizikal mekanikal akan berkurangan apabila suhu mencapai pada nilai optimum iaitu suhu 120Cf C. Komposisi formulasi yang terbaik adalah sampel G5T20 (5% sisa kaca dan 20% sisa jasad bakar ubin), manaka/a suhu pembakaran yang optimum ialah pada suhu 120Cf C. Melalui kajian ini, penggunaan campuran sisa kaca dan jasad bakar ubin mampu menghasilkan produk seramik untuk kegunaan di dalam bidang struktur seperti ubin /antai dan dinding, berdasarkan prestasi sifat mekanikal dan fizikal yang dipamerkan.

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ACKNOWLEDGEMENTS

First and foremost, I would like to take this opportunity to express my sincere acknowledgement to my supervisor Dr. Muhammad Zaimi bin Zainal Abidin from the Faculty of Manufacturing Engineering Universiti Teknikal Melaka (UTeM) for his essential supervision, support and encouragement towards the completion of this report.

I would also like to express my greatest gratitude to KKTM Masjid Tanah programme coordinator, Dr.Nur Izan Syahriah Binti Hussein from the Faculty of Manufacturing Engineering Universiti Teknikal Melaka (UTeM) for her effort and guidance.

Special thanks to MARA for giving full scholarship throughout this project. To Kolej Kemahiran Tinggi MARA Masjid Tanah Director, Mrs. Noresah Bt. Lani, Academic Deputy Director, Mr. Rahim Bin Selamat, Ceramic Processing Head Department, Mr. Khairul Anuar Bin Mohd. Jais and all KKTM Masjid Tanah staff for giving fully support during this study.

Particularly. I would also special thanks to Mr. Hairul Hisham, the technicians from material laboratory Faculty of Manufacturing Engineering for his assistance and efforts in XRD and particle size analysis works.

Special thanks to all my beloved, wife, sons and peers for their moral support in completing this degree. Lastly, thank you to everyone who had been to the crucial parts of realization of this project.

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DECLARATION APPROVAL DEDICATION ABSTRACT ABSTRAK ACKNOWLEDGEMENTS TABLE OF CONTENTS LIST OFT ABLES LIST OF FIGURES LIST OF APPENDICES LIST OF ABRREVIATIONS

CHAPTER

1. INTRODUCTION

1.1 Background of study

1.2 Problem statement

1.3 Research Questions

1.4 Aim and Objectives

1.5 Scope of study

TABLE OF CONTENTS

2. LITERATURE REVIEW

2.1 Introduction

2.2 Waste

2.3 Recycling waste

2.4 Glass

2.4.1 Composition and types of glasses

2.5 Rcycling of glass

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ii iii iv

viii ix xii xiii

1

1

2

3

3

5

6

6

6

7

8

8

11

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2.6 Ceramic Bodies 11

2.6.1 Porcelain 13

2.7 Raw Materials 14

2.7.1 Clay 15

2.7.2 Feldspar 17

2. 7 .3 Silica 17

2.7.4 Waste Materials 10

2.7.4.1 Categories ofwaaste in ceramic article 18

2.7.4.2 Glass waste 19

2.7.4.3 Grog 19

2.8 Mullite Formation 20

2.8.1 Mullite Formation in Porcelain 20

2.9 Effect of mixing composition on phase formation and properties 25

2.9.1 Grog in ceramic bodies 25

2. 9 .2 Glass waste in ceramic bodies 27

2.10 Effect of firing temperature on phase formation and properties 29

2.10.1 Phase formation and microstucture 29

2.10.2 Physical and mechanical properties 32

2.11 Uniaxial Powder Pressing 35

3. METHODOLOGY 36

3.1 Introduction 36

3.2 Raw materials 38

3.2.1 Waste raw materials 38

3.2.2 Porcelain formulation 40

3.3 Process Background 41

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3.3.1 Raw material and Samples Preparation 41

3.3.2 Firing 45

3.4 Testing and Analysis 46

3.4.1 Raw Material Characterisation and Analysis 46

3.4.2 Physical -Mechanical properties 47

3.4.3 Chemical, Phase and Microstructure Analysis 52

3.4.3. l Chemical composition analysis 52

3.4.3.2 Microstructure Analysis 52

3.4.3.3 Phase Analysis 54

4. RESULT AND DISCUSSION 55

4.1 Raw Material Characterization 55

4.1.1 Chemical composition 55

4. 1 .2 Mineralogy and phase analyis of raw materials 56

4.1.3 Thermal analysis of glass waste and fired tile 57

4.1.4 Particle size distribution 59

4.2 Fired Sample Characterization 61

4.2.1 Physical and mechanical properties 61

4.2.2 Shrinkage 64

4.2.3 Bulk density 65

4.2.4 Apparent porosity 67

4.2.5 Water absorption 68

4.2.6 Flexural strength or Modulus of Rupture (MOR) 70

4.3 Chemical Composition and Phase Analysis 72

4.3.1 Chemical Composition 72

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6.

4.4 Microstucture Analysis

4.4.1 Microstucture of porcelain with glass waste and grog

4.5 Thermal Analysis

4.6 Phase Analysis of Fired Sample

CONCLUSION AND RECOMMENDATIONS

6.1 Conclusion

6.2 Recommendations

REFERENCES

APPENDICES

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74

74

77

79

82

82

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84

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LIST OFT ABLES

TABLE TITLE PAGE

2.1 Chemical com_position of different types of glass 9

2.2 Traditional definition of Whiteware 12

2.3 Life history of a triaxial body 22

2.4 Results ofRietveld-RIR Quantitative Analysis 29

3. 1 Chemical composition of glass and fir~ tile 3-8

3.2 Reformulation composition of porcelain body 40

4.0 Chemical composition of the raw materials 56

4.1 Mineralogy and phase analysis of raw material 57

4.2 Particle size distribution of raw materials 60

4.3 Particle size distribution of mixing porcelain bodies 60

4.4 Average data of physical and mechanical properties of 63 sample

4.5 -ChemfoaJ composition sample before firing 73

4.6 Chemical composition sample at l l 50°C 73

4.7 Chemical composition sample at l 200°C 74

4.8 Mineralogy phase of the sample G5T20atl150°C, 1200°C, 80 l 250°C and l 280°C

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LIST OF FIGURES

TABLE TITLE PAGE

2.1 Composition of solid waste in Malaysia 7

2.2 Phase diagram ofK20.Ah03.4Si02 system 13

2.3 Schematic illustration of the suggested microstructural 23 evolution in triaxial porcelain

2.4 Box diagram of suggested phase evolution in triaxial 24 porcelain

2.5 Change in phase composition in function of firing 30 temperature

2.6 Microstucture and EDX analysis in SEM pbotomicograpb of 31 Tradiational Porcelain at 1340°C

2.7 Microstucture and EDX analysis in SEM photomicograph of 32 Glass Powder Porcelain at 1240°C

2.8 Effect of firing temperature on water absorption and linear 33 shrinkage

2.9 Effect of firing temperature on modulus of rupture 34

2.10 Effect of firing temperature on d_ensity 34

2.11 The scheme of the die pressing method 35

3.1 Research activity process flow 37

3.2 Window glass waste 39

3.3 Fired ceramic tile scrap 39

3.4 Fired ceramic wall tile macrostucture 40

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3.5 Disc crusher 41

3.6 Porcelain jar mill for mixing and milling 42

3.7 Process flow for powder preparation 43

3.8 Automatic hydraulic laboratory pressing machine 44

3.9 Firing profile 45

3.10 Dilatometer 47

3.11 Water bath for water absorption and apparent porosity 49

3.12 Density balance for bulk density 50

3.13 Universal testing machine, UTM 51

3.14 Bench-top X-ray fluorescence(XRF) analyser 52

3.15 Optic Microscope wih image capture 53

4.1 Thermal analysis of glass waste 58

4.2 Thermal analysis of fired ceramic tile 58

4.3 Pellet samples by different temperature and formulation for 61 physical properties characterization

4.4 Bar samples for flexural strength test 62

4.5 Linear shrinkage 65

4.6 Bulk density 66

4.7 Apparent porosity 67

4.8 Water absorption of porcelain at different firing temperature 69

4.9 The effect of amount waste in porcelain on water absorption 69 at 1200°C

4.10 Modulus of rupture of samples at different ftring and waste 71 composition

4.11 The effects of firing temperature in G5T20 sample on 71 Modulus of Rupture and Apparent Porosity

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4.12 Photograph of micro structure G 15T 10 at (a) l 250°C (b) 75 1280°C

4.13 Photograph of microstructure (xlO) (a) G 15TIO and (b) 76 G20T5 at 1280°C

4.14 Photograph ofmicrostructure of G5T20 (a) 1150°C (b) 76 1200°C (c) 1250°C and (d) 1280°C (xlOO)

4.15 Coeficient of thermal linear expansion of fired samples 78 firing at 1200°C

4.16 X-Ray diffraction pattern: (a) SP,1200°C, (b) 81 G5T20,1150°C, (c) G5T20,1200°C, (d)G5T20, 1250°C ( M:mullite, Q:quartz, P:plagioclase)

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APPENDIX

A

B

c

D

E

LIST OF APPENDICES

TITLE

Ghantt Chart (Research Milestone)

International Standard, ISO 13006 Ceramic tiles-Definition, classification,characteristics and marking

ASTM C 373-88

X-Ray Fluoresence, XRF data for raw materials

Particle size distribution data for raw materials

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LIST OF ABBREVIATIONS

Lo Dry length

L1 Fired length

WA Water absorption

Ms Soak weight

Mr Fired weight

W1 Dry weight

W2 Suspension weight

W3 Wet weight

F Force

b Width

h Thickness

D,d Diameter

BD Bulk Density

MOR Modulus of Rupture

UTM Universal Testing Machine

XRD X-Ray Diffraction

XRF X-Ray Fluorescence

SEM Scanning Electron Microscope

CTE Coefficient of Thermal Expansion

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CHAPTER I

INTRODUCTION

1.1 Background of Study

Recycled materials have now become a part of the processing stream, taking the

place of virgin materials in manufacturing. Manufacturing with recycled materials can

reduce cost conserves raw materials and reduces energy consumption. Porcelain is a

triaxial whiteware that is composed mainly of quartz, feldspar and kaolin. Feldspar is the

most expensive raw material and therefore its replacement would represent a significant

reduction in final costs. Feldspar is a fluxing agent used to reduce the firing temperature.

This fluxing agent can be replaced by using inexpensive material such as the glass waste

(Youssef et. al., 1998, Matteucci et. al., 2002) and granite waste (Vieira et. al., 2004). The

glass waste component in municipal waste is usuaJly made up of window glass, bottles,

broken glassware, light bulbs and other items. Chemical composition of glass waste (soda­

lime glass) is composed of alkaline silicate which can react as fluxing agent to reduce the

firing temperature. Fired glazed tile will be replacing the quartz partially. The function of

fired glazed tile in ceramic body as filler, where usually exhibited by quartz or silica. This

work is based on this fact and investigates the use of milled powder obtained from recycled

soda- lime glass as a fluxing agent and grog ( frred glazed tiles) act as filler for porcelain.

Reformulation of the new porcelain body incorporated with waste material were prepared

and processed under the same experimental conditions so as to make the data more

comparable.

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There are various types of forming techniques of ceramic products such as wet

pressing, powder pressing and slip casting. In this study uniaxial pressing is chosen as a

method for compaction and shaping of the powder materials into a green compact body.

Subsequently, green compact body then has been dried and fired in a furnace to develop

the desired microstructure and properties. This stage is also called sintering which involve

the shrinkage and densification. The performance of the final product will be analysed in

terms of its microstructures, phase's present and physical-mechanical properties. In this

study, Scanning electron microscope (SEM) and x-ray diffraction (XRD) analysis are used

to analyse the microstructure and phases present in the samples produced. Physical

analysis and mechanical testing are also conducted in order to analyse the properties of the

samples.

1.2 Problem Statement

Currently eco-material or sustainable manufacturing a major focus in the

manufacturing industry. Demand and marketability of eco-friendly products is a key aspect

of research in the use of waste materials. Recyclable waste material will _reduc_e _the

environmental impact, through lowering the amount of residues or treating those that are

inevitably generated during production processes. High costs associated with raw material

extraction, as well as the damage that the extraction causes to the environmen4 are also

important reasons to motivate the use of industrial process residues. Glass waste and tiles

were one of the waste materials be produced either in the field of building, constructions

and consumer domestic. Recycling glass has big environmental pay offs. It saves raw

materials, lessens demand for energy, and cuts C02 emissions. Reject tiles and unsold tile

is one reason dumping tile at the landfill. Therefore, if these waste glass and tiles are used

in ceramic products, the pollution of environmental can be decreased. Many studies have

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been made to use the glass waste ( cullet) as a raw material such as in the production of

glass container, bricks (Dondi et. al. , 2009) and tiles (Luz, et. al., 2007, and Matteuci, et.

al., 2002) as a fluxing agent. However, the use of waste glass as an alternative raw material

for fluxing agent may have an impact on the end product properties, such as strength,

density and water absorption. In the porcelain a necessary phase in mullite phase, because

the phase mullite be the major factor in determining the strength of porcelain bodies.

Studied by Mahmoud et. al., (2006) found that the increasing of mullite phase in hard

porcelain lead to increasing density, hardness, bending strength and decreasing the

porosity. Lee et. al., (2001) said various types of mullite is strongly dependent on the

extent of mixing of the body raw materials. From Y aseen et. al., (2000) primary mullite

fonns from decomposition of pure clay (primary mullite forms at 1000 °C) and secondary (

granular type-II and elongated type-III) mullite by reactions of clay and feldspar and clay,

quartz and feldspar ( forms at > l 200°C). Secondary mullite phase is the major contributor

to the quality of the properties of porcelain (hardness, bending strength ). Loryuenyong et.

al., (2012) found that the secondary mullite (mullite needles) gives high mechanical

strength and thermal shock resistance to porcelain body. Support by Dondi et. al., (1995)

that a higher mullite content contributes to a higher mechanical strength. Alumina shortage

in glass waste can inhibit the formation of mullite phases, thus fired tile scrap added to the

sample to provide Al203 element. Additional fired tiles scrap into the porcelain bodies will

helpfully assist the formation of mullite phase, and thus increase the technological

properties of porcelain. The purpose of the present study was to investigate the effect of the

additional of glass waste and fired tile scrap on mullite phase formation and evolution of

physical and mechanical properties of porcelain.

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t.3 Research Questions

In this present research, the answer to this question was investigated.

1. Can the mixture of waste glass and scrap of glazed tile be used in porcelain

body?

ii. Can the glass waste and scrap of glazed tiles as a raw material in porcelain

a better behaviour sintering?

1.4 Aim and Objectives

The objective of this research is:

1. To prepare the new formulation of porcelain using waste materials (such as

glass waste and fired tiles)

ii. To characterize the physical-mechanical properties of porcelain with

different percentage of waste material at different firing tempe.rature.

m. To analyse the microstructure of porcelain due to different percentages of

waste material.

1.5 Scope of Study

This study focuses on physical and mechanical properties behaviour of porcelain

bodies mixture with glass waste and grog (fired ceramic tiles scrap). The fabrication

process is by uniaxial powder pressing method. The study starts by preparing recycle glass

and scrap fired tiles as raw materials to be used in fabrication of porcelain samples. The

glass waste powders were prepared by crushing plate glass (window glass) made from the

disc crusher and milling until they passed through a sieve of less than 100 µm to obtain

fine particles .Reformulation porcelain added waste mixed in ball mill and screened

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through a sieve 63 µm. The powder was prepared by mixing 8-10% water, before preparing

a sample pressed done. All the raw materials will be analysed using XRF and XRD to

identify their chemical composition and mineralogical phase. Particle size of waste

material also will be analysed. Fired product will be characterized through physical and

mechanical testing such as flexural test, water absorption, porosity, linear firing shrinkage

and bulk density. The result will be supported by various analysis techniques such as optic

microscope, SEM, XRF and XRD. All experimental activities such as sample preparation,

testing and analyze planned on Gantt Chart (Appendix A). The effect of glass waste and

grog in different percentage in porcelain will be studied. In this study glass waste is used is

clear window glass. Grog will be used in this study is fired glazed wall ceramic tile.

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CHAPTER2

LITERATURE REVIEW

2.1 Introduction

The use of recyclable materials is the latest move to reduce the effects of pollution

to the environment. Waste materials selection should be based on the main functions of

each raw material us~_d in the formulation of p_ore:elain body. Every raw material waste

must undergo the characteriz.ation process early to ensure that the material does not cause

harmful effects such as the release of toxic gases or significantly reduce the quality or

nature of porcelain main body as strength, wate_r ~lls_Qmti_o_ll, _shrinka_ge, _bulk _density _and

others.

2.2 Waste

From National Solid Waste Management Department according Act 167 define of

solid waste includes any scrap material or other unwanted surplus substance or rejected

products srising from the application of any process; any substance required to be disposed

of as being broken, wom out, contaminated or otherwise spoiled; or any other material that

according to this Act or any other written law is required by the authority to be disposed of,

but does not include scheduled wastes as prescribed under the Environmental Quality Act

1974 (Act 127), sewage as defined in the Water Services Industry Act 2006 (Act 655) or

radioactive waste as defined in the Atomic Energy Licensing Act 1984 (Act 304). Based

on information from National Solid Waste Management Department, composition of solid

waste in Malaysia in 2005 as below:

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