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UNIVERSITI PUTRA MALAYSIA

PREPARATION AND CHARACTERIZATION OF Sr-YIG AND YIG-PVA

COMPOSITE

Mohd Shamsul Ezzad Shafie

FS 2009 54

PREPARATION AND CHARACTERIZATION OF Sr-YIG AND YIG-PVA COMPOSITE

BY

MOHD SHAMSUL EZZAD SHAFIE

FACULTY OF SCIENCE UNIVERSITI PUTRA MALAYSIA

August 2008

i


BY

MOHD SHAMSUL EZZAD SHAFIE

Thesis submitted to the School of Graduate Studies, Universiti Putra Malaysia,

in fulfilment of the requirement for the degree of the Master of Science

August 2008

ii

DEDICATION

I would like to dedicate this thesis to:

• My family members

‘Shafie Bin Awang, Norizah Bt Mat, Mohd

Shamsul Rizal and Siti Norhazlina’

For teaching me these words,

“Hidup adalah segugus pengalaman

yang mengajar kita menafsir

dan mengenal untung nasib

antara kebahagiaan

atau takdir yang rapuh

kita pasti terpalit warnanya”

iii

Abstract of the thesis presented to the Senate of Universiti Putra Malaysia in Fulfilment of the requirement for the degree of Master of Science


By


August 2008

Chairman : Associate Professor Dr. Mansor Hashim, PhD Faculty : Science

This thesis deals with the subject of magnetic properties

utilizing iron garnet materials. The main purpose of this project is to prepare

of Y3.0-XSrXFe5O12 and develop of YIG-PVA composite films. In addition, other

properties including Q-factor, microstructure and XRD had also been studied. For

powder preparation, seven garnet powder samples were prepared which are Y3.0-

XSrXFe5O12 (x = 0 to 2.5), in the interest of 0.5 value. From the results, the highest

permeability obtained at sample Y3.0Fe5O12 (YIG) which is 1.58. The lowest loss

factor is 7.41, which is obtained from sample Y1.5Sr1.5Fe5O12. From the XRD

characterization, the peak changing from 32.31° to 32.89°, indicating the transition

from YIG to Strontium based iron garnet. From the SEM analysis, the

Y2.0Sr1Fe5O12 has the largest grain size while Y3S0 exhibit smallest grain size. As a

conclusion, this sample can be utilized for high frequencies applications.

Considering the best microstructure, highest permeability, lower LF, the best sample

is YIG. It was chosen as filler in preparation polymer composite. For polymer

iv

composite preparation, the composites consisted of polyvinyl alcohol (PVA) and YIG

were prepared by casting technique. YIG (1 wt%) and YIG (5 wt%) prepared as

filler in polyvinyl alcohol (PVA) as polymer composite. Both YIG exhibit similar

XRD patterns to standard YIG sample including extra peak for PVA at 40˚.

Compared to YIG (1 wt%), the YIG (5 wt%) was more effective to improve the

magnetic properties of the composites because of its network structure. In

conclusion, a certain high level of filler content was proven to be necessary for the

promotion of magnetic properties in oriented composite.

v

Abstrak tesis yang dikemukakan kepada Senat Universiti Putra Malaysia sebagai memenuhi keperluan untuk ijazah Master Sains

PENYEDIAAN DAN PENCIRIAN Sr-YIG DAN YIG-PVA

KOMPOSIT

Oleh


Ogos 2008

Pengerusi : Professor Madya Dr. Mansor Hashim, PhD Fakulti : Sains

Thesis ini menjuruskan penyelidikan berkaitan bahan magnetik

menggunakan bahan garnet sebagai asasnya. Tujuan sebenar

penyelidikan ini adalah untuk menyediakan Y3.0-XSrXFe5O12 dan

menghasilkan polimer komposit YIG-PVA. Sebagai tambahan, ciri-ciri lain seperti

faktor-Q, mikrostruktur dan XRD juga telah dikaji. Untuk penyediaan hablur, tujuh

kumpulan serbuk bahan garnet telah disediakan secara formula, iaitu Y3-xSrx Fe5O12,

(x = 0 sehingga 2.5, dalam perbezaan nilai 0.5). Daripada penyelidikan, ketelapan

tertinggi diperolehi dari sampel Y3.0Fe5O12 (YIG) iaitu 1.58. Faktor kehilangan

terendah adalah 7.41, dimana diperoleh daripada sampel Y1.5Sr1.5Fe5O12. Daripada

pencirian XRD, puncak berubah daripada 32.31° ke 32.89°, menunjukkan peralihan

daripada YIG kepada Strontium berasaskan garnet. Daripada analisa SEM,

Y2.0Sr1Fe5O12 mempunyai saiz butiran terbesar manakala YIG mempamerkan saiz

butiran terkecil. Sebagai kesimpulan, sampel ini boleh digunakan untuk applikasi

frekuensi peringkat tinggi. Dengan mempertimbangkan mikrostruktur terbaik,

vi

ketelapan tertinggi, LF terendah, sampel terbaik adalah YIG. Ia telah dipilih sebagai

bahan isian dalam penyediaan polimer komposit. Untuk penyediaan polimer

komposit, komposit yang terdiri oleh polyvinyl alcohol (PVA) dan YIG telah

disediakan menggunakan kaedah tebaran daripada campuran YIG dan PVA. Daripada

analisa SEM, Y2.0Sr1Fe5O12 mempunyai saiz butiran terbesar manakala YIG

mempamerkan saiz butiran terkecil. Sampel ini boleh digunakan untuk aplikasi

frekuensi tinggi. Dengan mempertimbangkan butiran terbaik, ketelapan tertinggi,

factor kehilangan yang lebih rendah, sampel terbaik adalah sampel YIG dan ia dipilih

sebagai bahan isian dalam penyediaan polimer komposit. . YIG (1 wt%) dan YIG (5

wt%) disediakan sebagai bahan isian di dalam polyvinyl alcohol (PVA) sebagai

polimer komposit. Kedua-dua mempamerkan bentuk XRD yang serupa dengan

piawai sampel YIG termasuk puncak tambahan untuk PVA pada 40˚. Dibandingkan

dengan YIG (1 wt%), YIG (5 wt%) adalah lebih efektif untuk meningkatkan bahan

magnetik komposit kerana struktur jaringannya. Kesimpulannya, paras kandungan

bahan isian tertentu telah dibuktikan perlu untuk menggalakkan peningkatan magnetik

dalam orientasi komposit.

vii

ACKNOWLEDGEMENT

I would like to thank to all those who made it the possible for me to complete this

thesis. First of all I would like to express my gratitude to Associate Professor Dr.

Noorhana Yahya. She has always been extremely generous with her time and

knowledge, and allowed me great freedom in this research. It was a great pleasure

for me to conduct this thesis under her supervision. I also acknowledge Associate

Professor Dr. Mansor Hashim, who act as my co-supervisor provided helpful

suggestions toward the success of this thesis. I would like to thank the staff and

technicians of Bioscience Institute (IBS), specially Kak Ida, Faris, Mr. Ho, Aini and

Rafi, without whose help this work would not have been possible. Thank you for

your time and help with the SEM analysis. Great thanks also to Yusnita and

Yusmawati for helping me in running XRD for all my samples.

I am grateful to my colleagues who have collaborated with me at the Advanced

Material Laboratory, ITMA, particularly Hoe Guan, Ramadan, Liu, Samaila,

Ismayadi and Hashim. I appreciate your support and comments at all time. Not only

with the academic support which is important to conclude a thesis but also the

morale support especially when I am so far from home. I am deeply grateful to my

housemate and all friends for making me feel at home. There are no words to thank

my family for their love and support despite their distance from me. Thank you for

your prayers that always accompanying me. I would like to thank my close friend,

Sheikh Ahmad Izadin for being my mate of dreams, hopefulness and striving.

Thanks also for your help (borrowing laptop) and unconditional support. Finally but

certainly not least important, I am infinitely grateful to ALLAH for being my

fortitude and refuge.

viii

I certify that an Examination Committee met on 1 August 2008 to conduct the final examination of Mohd Shamsul Ezzad Shafie on his Master of Science thesis entitled “Preparation and characterization of Sr-YIG and YIG-PVA Composite” in accordance with Universiti Putra Malaysia (Higher Degree) Act 1980 and Universiti Putra Malaysia (Higher Degree) Regulations 1981. The Committee recommends that the candidate be awarded the relevant degree. Members of the Examination Committee are as follows: Ilias Saion, PhD Associate Professor Faculty of Science Universiti Putra Malaysia (Chairman)

Sidek Ab. Aziz, PhD Associate Professor Faculty of Science Universiti Putra Malaysia (Internal Examiner)

Zainal Abidin Talib, PhD Associate Professor Faculty of Science Universiti Putra Malaysia (Internal Examiner)

Sinin Hamdan , PhD Associate Professor Faculty of Science Universiti Malaysia Sarawak (External Examiner)

BUJANG KIM HUAT, PhD Professor and Deputy Dean School of Graduate Studies Universiti Putra Malaysia Date: 19 March 2009

ix

This thesis submitted to the Senate of Universiti Putra Malaysia has been accepted as fulfillment of the requirement for the degree of Master of Science. The members of the Supervisory Committee are as follows: Mansor Hashim, PhD Associate Professor Faculty of Science Universiti Putra Malaysia (Chairman) Noorhana Yahya, PhD Associate Professor Faculty of Science Universiti Putra Malaysia (Member) __________________________ HASANAH MOHD GHAZALI, PhD Professor and Dean Dean of Graduate School Universiti Putra Malaysia

Date: 9 April 2009

x

DECLARATION I hereby declare that the thesis is based on my original work except for quotations and citations which have been duly acknowledged. I also declare that it has not been previously or concurrently submitted for any other degree at UPM or other institutions. ________________________________ MOHD SHAMSUL EZZAD SHAFIE

Date:

xi

TABLE OF CONTENT Page ABSTRACT iii ABSTRAK v DEDICATION viii ACKNOWLEDGEMENT ix APPROVAL x DECLARATION xi LIST OF TABLES xvi LIST OF FIGURES xvii LIST OF SYMBOLS AND ABBREVIATIONS

xxi

LIST OF APPENDICES xxiii

CHAPTER 1. INTRODUCTION

1.1 Introduction 1 1.2 Ferrites 2 1.3 Garnet 4 1.4 Soft magnetic material and

their applications 6

1.4.1 Yttrium Iron Garnet (YIG) and its applications

8

1.5 Sol-gel 9 1.6 Aim 11 1.7 Objectives 11 1.8 Chapter organizer 11

2. LITERATURE REVIEW

2.1 Introduction 13 2.2 Background research on

Yttrium Iron Garnet at UPM and other researcher

13

2.3 History of Ferrites and Garnets 15 2.3.1 Synthesis and Characterization

of Yttrium Iron Garnet Nanoparticle

15

2.3.2 Magnetic Properties 19 2.3.3 Low temperature sintering of

microwave magnetic garnet materials

20

2.3.4 Influence of Substitution of Magnesium and Calcium in YIG and Bi-YIG

21

2.4 Polyvinyl Alcohol (PVA) 22

2.5 Current study on ferrite-

polymer composite 23

xii

3. THEORY

3.1 Introduction 26 3.2 Theory of Garnet 26

3.2.1 Structure of garnet 26 3.3 Wet Chemical Preparation

Methods 29

3.4 Theory of Sol-Gel Method 31 3.4.1 Sol gel technique 31

3.5 Theory of X-ray Diffraction 36 3.5.1 Lattices Planes and Bragg’s

Law 36

3.5.2 Diffraction 39 3.5.3 Magnetism 41

3.6 Magnetic Domains 46 3.7 Magnetic Properties of Ferrites

Studied in This Research 47

3.7.1 Permeability 47 3.7.2 Magnetic losses 48 3.7.3 Grain Size 49 3.7.4 Quality Factor (Q- factor) 50 4. METHODOLOGY

4.1 Introduction 52 4.2 Preparation of Yttrium Iron

Garnet substituted Strontium 53

4.2.1 Raw materials 54 4.2.2 Weighing 54 4.2.3 Mixing 55 4.2.4 Drying 55 4.2.5 Pre-sintering 55 4.2.6 Crushing and Grinding 56 4.2.7 Addition of Binder and

Lubricant (Granulation) 57

4.2.8 Moulding 57 4.2.9 Sintering 58

4.3 Polymer composite preparation

59

4.3.1 Addition of PVA and Homogeneous Mixing for 2 Hours

59

4.3.2 Cutting and Hydraulic Pressing (Moulding)

59

4.4 Physical Characteristics Measurement

60

4.4.1 XRD Measurement 60 4.4.2 Diameter and Height 60 4.4.3 Density measurement 61

xiii

4.4.4 Shrinkage 61 4.4.5 Complex Permeability 62 4.4.6 Magnetic Losses Measurement 63 4.4.7 Scanning Electron Microscopy

(SEM) Analysis 63

5. RESULTS AND

DISCUSSION

5.1 Introduction 64 5.2 XRD Characterization 64 5.3 Shrinkage 78 5.4 Microstructure 80 5.5 Magnetic Analysis

Measurement 87

5.5.1 Q-Factor 87 5.5.2 Permeability 89 5.5.3 Loss Factor 92

5.6 Polymer Composite 93 5.6.1 Dimension 93 5.6.2 XRD 94 5.6.3 Magnetic properties 98 5.6.4 Treatment with liquid

Nitrogen 105

5.6.4.1 Polyvinyl Alcohol (PVA) (5%)

105

5.6.4.2 PVA composite filled Y3S0 (5%)

106

5.6.5 Energy Dispersive X-Rays (EDX)

110

6. CONCLUSION AND

SUGGESTION

6.1 Conclusion 114 6.2 Suggestions 116

BIBLIOGRAPHY 117

APPENDICES 123

BIODATA OF STUDENT 157

xiv

LIST OF TABLES

Table Page

3.1 List of values of h2+ k2+ l2 equated with their hkl values 38

4.1 Weight of the raw materials used in this work 54

5.1 Count/s and respective 2 Theta [degree] for every sample at 600˚C 65







5.8 Shrinkage (%) for every toroidal sample at 800˚C 78

5.9 Q factor at four different frequencies for all samples 88

5.10 Dimension for theY3S0 samples 93

5.11 EDX result of 1% YIG polymer composite 111

5.12 EDX result of 5% YIG polymer composite 113

xv

LIST OF FIGURES

Figure Page

3.1 Arrangement of cations in a garnet structure. Positions 3-- c, 1-- a,

2-- d

28

3.2 Coordination around an oxygen ion garnet 1--- O2+, 2--- Al3+,

3--- Si4+, 4--- Ca2+

28

3.3 Different method in ceramic processing 30

3.4 Acid- Catalyzed Reaction 33

3.5 Base- Catalyzed Reaction 33

3.6 Sol-gel process and microstructure of sol-gel products 34

3.7 The planes of a crytal 37

3.8 The reflection of an X-ray beam 37

3.9 Schematic illustration of the reflection of an x-ray beam by the

planes of a crystal

40

3.10 Schematic of Magnetic Moments Ferromagnetism 45

3.11 Schematic of Magnetic Moment Ferrimagnetism 45

3.12 Schematic of Magnetic Moment Antiferromagnetism 45

3.13 Magnetic Domains 46

3.14 Schematic Representation of Magnetic Domains 47

4.1 Sol-gel technique flow chart for polymer composite preparation 54

4.2 Heating and cooling rate during the final sintering 58

4.3 Measuring Sample’s Weight in Air and Water 61

4.4 Dimension of Toroidal shape 62

5.1 XRD patterns of each samples where are annealed at 600°C 65



xvi





5.8 Densities (%) Vs Mole Fraction of Strontium 79

5.9 Microstructure of Y3S0 81

5.10 Microstructure of Y2.5S0.5 81






5.16 Q factor for every sample at 800°C sintering temperature 87

5.17 Q factor for every sample at four different frequency ranges 87

5.18 Real permeability for every sample at 800°C 90

5.19 Q factor for Y3S0, Y2.5S0.5 and Y2S1 Vs mole fraction of Sr2+ 90

5.20 Loss factor for every sample at 800°C 92

5.21 XRD patterns for Polyvinyl Alcohol (PVA) 95

5.22 XRD patterns for Y3S0 (1%) polymer composite 95

5.23 XRD patterns for Y3S0 (5%) polymer composite 96

5.24 Q factor for sample pure PVA and Y3S0 [1% and 5%] polymer

composite

98

5.25 Real permeability for pure PVA and Y3S0 [1% and 5%] polymer

composite

99

5.26 Loss factor for pure PVA and Y3S0 [1% and 5%] polymer

composite

102

xvii

5.27 Polyvinyl Alcohol (PVA). [a] 105

5.28 Polyvinyl Alcohol (PVA) [b] 105

5.29 Polymer composites filled YIG nanoparticles 106

5.30 The dispersion of YIG nanoparticles in PVA film 106

5.31 Closer image of YIG in PVA film 107

5.32 The average size of YIG particles in PVA film 107

5.33 Y3S0 (5 wt%). dispersed pattern for first spectrum in PVA 110

5.34 Element dispersed for polymer composite first spectrum 110

5.35 Y3S0 (5 wt%). dispersed pattern for second spectrum in PVA 112

5.36 Element dispersed for polymer composite second spectrum 112

xviii

LIST OF SYMBOLS AND ABBREVIATIONS

Symbol

Greek Symbol

μ permeability of ferrite core

μi initial permeability

μ′ real part of permeability

μ″ imaginary part of permeability

μo permeability of free space

μr relative permeability of material

μB The Avogadro or Loschmidt number

tan δ loss tangent

tan δtot total loss tangent

π pi (22/7)

γ gyromagnetic ratio

τ relaxation time s

θ theta oC

ω angular frequency Hz

λS average point of magnetostriction m

αx directional cosines

θB Bragg’s Angle

λ wavelength of electromagnetic wave m

ε subsequent path

φ phase difference

xix

LIST OF SYMBOLS AND ABBREVIATIONS

Symbol

Other Symbol

Do outer diameter of film meter

Di inner diameter of film meter

t thickness of film meter

f measured frequency Hertz

fr resonance frequency Hertz

H magnetic field Oersted or A/m

B magnetic induction Gauses or Teslas

(werbers / m2)

c velocity of light in free space m /s2

Rs series loss resistance ohm

Ls series inductance Henry

Δ(2θ) Difference in 2θ angles / Line Breadth XRD X-Ray Diffraction

xx

xxi

LIST OF APPENDICES

Appendix Page

A Measurement: molecular weight for preparation on Y3.0Fe5O12

[Y3S0] and polymer composites

123

B Standard XRD data for Y3.0Fe5O12 [YIG] 125

C XRD Results for the sintered Samples for Y3.0Fe5O12 [Y3S0] 128

D XRD Results for the sintered Samples for Y2.5Sr 0.5Fe5O12

[Y2.5S0.5]

131

E XRD Results for the sintered Samples for Y2.0Sr 1.0Fe5O12 [Y2S1] 134

F XRD Results for the sintered Samples for Y1.5Sr 1.5Fe5O12

[Y1.5S1.5]

137

G XRD Results for the sintered Samples for Y1.0Sr 2.0Fe5O12 [Y1S2] 140

H XRD Results for the sintered Samples for Y0.5Sr 2..5Fe5O12

[Y0.5S2.5]

143

I XRD Results for the sintered Samples for Sr 3.0Fe5O12 [Y0S3] 146

J XRD Results for the sintered Samples for Y3.0Fe5O12 [Y3S0

(1wt%)]

149

K XRD Results for the sintered Samples for Y3.0Fe5O12 [Y3S0

(5wt%)]

152

1

CHAPTER 1

INTRODUCTION

1.1 Introduction

Nine years of worldwide revolutionary developments in nanoscience, combining

physics, chemistry, material science, theory and even biosciences, have brought us to

another level of understanding. Nanotechnology becomes a key word of public

interest, since even politician and economists realized the social power of

nanotechnological development. Nanotechnology is called the technology of the

next century, coming after microtechnology. Nanotechnology unfortunately also

becomes a catchword for people with ambitions in science fiction.

Nanoparticles themselves had been around and studied long before the words were

coined. For example, many of the beautiful colors of stained glass windows are

result of the presence of small metal oxide clusters in the glass, having a size

comparable to the wavelength of light. Particle of different sizes scatter different

wavelength of light, imparting different colors to the glass. Small colloidal particles

of silver are a part of the process of image formation in photography. Water at

ambient temperature consists of clusters of hydrogen-bonded water molecules.

Nanoparticles are generally considered to be a number of atoms or molecules bonded

together with a radius of <100nm. A nanoparticles is 10-9 m or 10Å, so particles

having a radius of about ≤1000Å can be considered to be nanoparticles.

2

1.2 Ferrites

The history of ferrites (magnetic oxides) and their applications have been known for

several centuries ago. The loadstone (magnetite, Fe3O4), a natural non-metallic solid,

may attract iron was first described in known Greek writings about 800 B.C. Much

later, the first application of magnetite was as 'Lodestones' used by early navigators

to locate magnetic North. That is the first scientific significance was appreciated,

after the first technical magnetic material because it formed the first compass

(Crangle, 1977). The first scientific study of magnetism named De Magnete was

published by William Gilbert in 1600. Later, in 1819 Hans Christian Oersted

observed that an electric current in a wire affected a magnetic compass needle.

Naturally occurring magnetite is a weak 'hard' ferrite. 'Hard' ferrites possess a

magnetism which is essentially permanent. Originally manufactured in a few select

shapes and sizes, primarily for inductor and antenna applications, 'soft' ferrite has

proliferated into countless sizes and shapes for a multitude of uses. Furthermore,

ferrites are used predominately in three areas of electronics: low level applications,

power applications, and Electro-Magnetic Interference (EMI) suppression. The

breadth of application of ferrites in electronic circuitry continues to grow. The wide

range of possible geometries, the continuing improvements in material characteristics

and their relative cost-effectiveness make ferrite components the choice for both

conventional and innovative applications.

3

Basically, ferrites are ceramic materials, dark grey or black in appearance and very

hard and brittle. Ferrites may be defined as magnetic materials composed of oxides

containing ferric ions as the main constituent (the word ferrite comes from the Latin

“ferrum” for iron) and classified as magnetic materials because they exhibit

ferrimagnetic behavior. The ferrites, in powder or thin film forms, can be prepared

by high-temperature solid-state reaction method, sol–gel method, coprecipitation,

pulsed laser deposition, high-energy ball milling and hydrothermal technique.

A ferrite core is made by pressing a mixture of powders containing the constituent

raw materials to obtain the required shape and then converting it into a ceramic

component by sintering. The magnetic properties arise from interactions between

metallic ions occupying particular positions relative to the oxygen ions in the crystal

structure of the oxide. In the commercial ferrites, they can be divided into three

important classes, with each one having a specific crystal structure, namely:

1. Soft ferrite with the garnet structure such as the microwave ferrites (e.g:

YIG).

2. Soft ferrites with the cubic spinel structure such as NiZn-, MnZn-, and

MgMnZn ferrites.

3. Hard ferrites with the magnetoplumbite (hexagonal) structure such as Ba and

Sr hexaferrites.

Ferrites are widely used in transformer and inductors for telecommunications, power

conversion and interference suppression. Much of the ferrite-related research took

place after the 1950s, thanks to a technology expansion in the fields of radio,

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