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UNIVERSITI PUTRA MALAYSIA EFFECT OF ULTRASONIC IRRADIATION ON LANDFILL LEACHATE CHUA SZE YE FPAS 2010 9

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UNIVERSITI PUTRA MALAYSIA

EFFECT OF ULTRASONIC IRRADIATION ON LANDFILL LEACHATE

CHUA SZE YE

FPAS 2010 9

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EFFECT OF ULTRASONIC IRRADIATION ON LANDFILL LEACHATE

By

CHUA SZE YE

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

in Fulfilment of the Requirements for the Degree of Master Science

April 2010

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Abstract of thesis presented to the Senate of Universiti Putra Malaysia in fulfilment of the

requirement for the degree of Master Science

EFFECT OF ULTRASONIC IRRADIATION ON LANDFILL LEACHATE

By

CHUA SZE YE

April 2010

Chair: Puziah Abdul Latif, PhD

Faculty: Environmental Studies

Landfilling method for the ultimate disposal of municipal solid waste material continues to be

widely accepted and used due to its economic advantages of decomposition in a landfill. Landfill

leachate is a type of wastewater which contains high concentration of organics which are

difficult-to-treat with conventional treatment methods such as biological methods due to the

presence of high fraction of molecular weight compounds and refractory organics. Ultrasonic

irradiation was selected due to its several advantages which include elimination on the use of

chemical oxidants for the treatment of complex organic compounds, shorter reaction time, etc.

The 20 kHz ultrasonic-induced reduction of chemical oxygen demand (COD) and total

suspended solids (TSS) were investigated. Several operating conditions, such as power density

(24 – 188 W/L), pH (2 – 11), dilution factor (1:9, 1:1 and 9:1), addition of different types and

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amount of catalyst (FeSO4 and CuSO4, 1.0 - 5.0 mmol/L and H2O2, 0.1 mmol/L) and powdered

activated carbon (PAC, 1 - 6 g), were tested to study their effect on COD and TSS percentage

reduction. Sample mineralization in term of COD and the particle rupture assessed by TSS were

investigated. The optimum conditions from the operating systems were then selected together

with by adding 2 g of powdered activated carbon which includes PAC/US, H2O2/PAC/US,

FeSO4/PAC/US and CuSO4/PAC/US systems. Combination of ultrasonic and other treatment

methods such as ultraviolet irradiation were also tested for its effectiveness in combination with

ultrasonic irradiation. The treatment methods were also added with 2 g of powdered activated

carbon. Overall, the best and optimum condition for the reduction of COD and TSS was PAC/US

system with the reduction of 97.26 % and 65.00 %. The percentage reductions were enhanced at

increased applied power densities (188 W/L), pH 7.4 (natural pH), initial leachate concentration

and 2 g of PAC. The percentage reductions of the two parameters were as high as 97.26 %

(PAC/US system) for COD and 87.64 % (H2O2/PAC/US) for TSS. Ultrasonic irradiation was

shown to be an effective method for the reduction of COD and TSS. The total mineralization of

organic pollutants by means of ultrasound irradiation alone and addition of catalysts still remains

a difficult task especially for high strength wastewater such as leachate. Ultrasonic pre-treatment

followed by other techniques, such as biological treatment or sonication coupled with other

oxidation techniques seems to be a promising method to treat leachate in order to develop an

economically more favorable integrated technique.

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Abstrak tesis yang dikemukakan kepada Senat Universiti Putra Malaysia sebagai memenuhi

keperluan ijazah Master Sains

KESAN SINARAN ULTRASONIK KE ATAS CECAIR LUPUSAN SAMPAH

Oleh

CHUA SZE YE

April 2010

Pengerusi: Puziah Abdul Latif, PhD

Fakulti: Pengajian Alam Sekitar

Kaedah pemendaman untuk pembuangan akhir bahan sisa pepejal terus diterima dan digunakan

secara meluas disebabkan manfaat ekonomi. Cecair lupusan sampah adalah sejenis cecair yang

mempunyai kepekatan organik yang tinggi dan sukar dirawati dengan kaedah konvensional

seperti kaedah biologi kerana terdapat sebahagian daripada cecair ini yang mempunyai berat

molekul pecahan tinggi dan sebatian organik refraktori. Kaedah rawatan secara sinaran

ultrasonik telah dipilih disebabkan oleh beberapa keuntungan yang meliputi penghapusan

penggunaan bahan oksidan kimia untuk rawatan sebatian organik kompleks, masa tindakbalas

yang lebih singkat dan sebagainya. Penggunaan gelombang ultrasonik 20 kHz untuk

mengalakkan pengurangan keperluan oksigen kimia (COD) dan jumlah pepejal terampai (TSS)

telah dikaji. Beberapa keadaan operasi, seperti kepadatan kuasa (24 - 188 W/L), pH (2 - 11),

kepekatan (1:9, 1:1 dan 9:1), penambahan pelbagai jenis dan jumlah mangkin (FeSO4 dan

CuSO4, 1.0 - 5.0 mmol/L dan H2O2, 0.1 mmol/L) dan serbuk karbon teraktif (PAC, 1 - 6 g) telah

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diuji mengenai keberkesanannya untuk peratusan penurunan nilai COD dan TSS. Pemineralan

sampel dalam sebutan pengurangan COD dan pecahan zarah dalam sebutan TSS juga telah

dikaji. Keadaan optima dari operasi tersebut kemudiannya telah dipilih dan ditambah dengan 2 g

serbuk karbon teraktif yang meliputi PAC/US, H2O2/PAC/US, FeSO4/PAC/US dan

CuSO4/PAC/US. Gabungan ultrasonik dan kaedah rawatan lain seperti sinaran ultra lembayung

juga telah diuji untuk menilai keberkesanannya bagi kombinasi dengan ultrasonik. Kaedah

rawatan juga ditambah dengan 2 g serbuk karbon teraktif. Secara keseluruhan, keadaan terbaik

dan optima bagi pengurangan COD dan TSS adalah sistem PAC/US dengan penurunan 97.26 %

dan 65.00 %. Peratusan penurunan kedua-dua parameter COD dan TSS meningkat pada

peningkatan kepadatan kuasa (188 W/L), pH 7.4 (pH semulajadi), kepekatan dan 2 g PAC.

Pengurangan peratusan dari dua parameter tersebut adalah setinggi 97.26 (sistem PAC/US) %

bagi COD dan 87.64 % (H2O2/PAC/US) bagi TSS. Hasil kajian menunjukkan sinaran ultrasonik

adalah kaedah yang berkesan untuk pengurangan COD dan TSS. Pemineralan jumlah pencemar

organik dengan cara sinaran ultrasonik sendirian dan penambahan pemangkin masih merupakan

satu masalah yang sukar untuk diatasi terutama untuk air kumbahan kekuatan tinggi seperti

cecair sampah. Pra-rawatan ultrasonik diikuti dengan teknik-teknik lain, seperti rawatan biologi

atau gabungan sonikasi dengan kaedah pengoksidaan yang lain mungkin berupaya bagi

menghasilkan satu teknik integrasi yang lebih menjimatkan.

ACKNOWLEDGEMENT

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First and foremost, I would like to express my sincere appreciation to my supervisor, Dr. Puziah

Abdul Latif and co-supervisor, Assoc. Prof. Dr. Shaharin Ibrahim for their invaluable help,

encouragement and advice throughout my research work. Their helpful comment always guides

me to solve the problem during my experiment to make this project successful.

I am deeply indebted to Dr. Mohd Roslan Mohamad Karim for his invaluable advice and

assistance that has contributed substantially in my thesis writing. I am grateful to the officer of

Alam Flora who helped me in the field work. His patience, helpfulness and sense of humor make

my field work an enriching experience. My heartfelt thanks, gratitudes and appreciate to my

research colleagues, Liza, Yee Jun, Fida, Norhidayah, Shamala and Ng Tung Yan for their

constant support, faith, endurance, understanding and encouragement which they have always

given me and make my thesis a very memorable one.

I also acknowledge the financial support from FRGS (5523056) on this project and UPM for

awarding the GRF. Last but not least, I would like to thank my parents and family members for

their warm encouragement and support. No brief mention can adequately convey my

appreciation to these people, but I hope the outcome warrants their support.

I certify that a Thesis Examination Committee has met on 21st April 2010 to conduct the final

examination of Chua Sze Ye on her thesis entitled “Effects of Ultrasonic Irradiation on Landfill

Leachate” in accordance with the Universities and University Colleges Act 1971 and the

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Constitution of the Universiti Putra Malaysia [P.U.(A) 106] 15 March 1998. The committee

recommends that the student be awarded the degree of Master of Science.

Members of the Thesis Examination Committee were as follows:

AHMAD MAKMOM ABDULLAH, PhD

Associate Professor,

Faculty of Environmental Studies

Universiti Putra Malaysia

(Chairman)

ABDUL HALIM ABDULLAH, PhD

Associate Professor,

Faculty of Science

Universiti Putra Malaysia

(Internal Examiner)

MOHAMAD PAUZI ZAKARIA, PhD

Associate Professor,

Faculty of Environmental Studies

Universiti Putra Malaysia

(Internal Examiner)

MAKETAB MOHAMED, PhD

Associate Professor,

Faculty of Chemical and Natural Resources Engineering

Universiti Teknologi Malaysia

(External Examiner)

____________________________

BUJANG BIN KIM HUAT, PhD

Professor and Deputy Dean

School of Graduate Studies

Universiti Putra Malaysia

Date: 23 July 2010

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This thesis was submitted to the Senate of Universiti Putra Malaysia and has been accepted as

fulfilment of the requirement for the degree of Master of Science. The members of the

Supervisory Committee were as follows:

PUZIAH ABDUL LATIF, PhD

Lecturer

Faculty of Environmental Studies

Universiti Putra Malaysia

(Chairman)

SHAHARIN IBRAHIM, PhD

Associate Professor

Faculty of Environmental Studies

Universiti Putra Malaysia

(Member)

_______________________________

HASANAH MOHD GHAZALI, PhD

Professor and Dean

School of Graduate Studies

Universiti Putra Malaysia

Date: 12 August 2010

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DECLARATION

I declare that the thesis is my original work except for quotations and citations which have

been duly acknowledged. I also declare that it has not been previously, and is not

concurrently, submitted for any other degree at Universiti Putra Malaysia or at any other

institution.

__________________

CHUA SZE YE

Date: 11 June 2010

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TABLE OF CONTENTS

Page

ABSTRACT ii

ABSTRAK iv

ACKNOWLEDGEMENT vi

APPROVAL vii

DECLARATION ix

LIST OF TABLES xi

LIST OF FIGURES xii

LIST OF ABBREVIATIONS xiv

CHAPTER

1. INTRODUCTION 1

1.1. General Introduction 1

1.2. Problem Statement 3

1.3. Research Objectives 4

1.4. Scope and Limitation of Study 5

1.5. Significance of Study 6

2. LITERATURE REVIEW 9

2.1. Solid Waste Management in Malaysia 9

2.2. What is Landfill Leachate? 10

2.3. Landfill Leachate Characteristics 11

2.4. Environmental Impact of Leachate 13

2.5. Current Method of Treating Leachate 14

2.5.1. Biological Treatment 15

2.5.2. Physical/Chemical Treatment 16

2.6. History of Ultrasound 17

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2.7. Advanced Oxidation Processes (AOPs) 17

2.8. Sonochemistry 19

2.9. Basic Principles of Sonochemistry 19

2.9.1. Acoustic Cavitation 19

2.9.2. Different Theories of Sonochemistry 23

2.9.3. Factor Affecting Sonochemical Reactions 23

2.10. Ultrasonic System Types 26

2.10.1. Ultrasonic Probe System 26

2.10.2. Ultrasonic Bath System 27

2.11. Other Application of Ultrasonic Irradiation 27

2.12. Combined process between Ultrasonic Irradiation, Catalysts,

Activated Carbon or other Treatment Technologies 28

2.12.1. Activated Carbon (Adsorption) 28

2.12.2. Catalysts 29

2.12.3. Combination of US and other Advanced Oxidation

Processes 31

2.13. Disadvantages of Ultrasound 32

2.14. Cost Estimation 33

3. METHODOLOGY 34

3.1. Introduction to Methodology 34

3.2. Materials 37

3.2.1. Collection of Landfill Leachate 37

3.2.2. Chemical/Reagent/Solvent Used 38

3.2.3. Method of Chemical Analysis for Water Quality

Parameters of Raw Leachate and Treated Leachate 39

3.2.4. Heavy Metal Analysis 40

3.3. Equipment Used 41

3.3.1. Treatment of Leachate Using Ultrasonic Probe only

at Varying Conditions 42

3.4 Statistical Analysis 49

4. RESULTS AND DISCUSSION 51

4.1. Effect of Power Density 51

4.2. Effect of pH 53

4.3. Effect of Dilution Factor 56

4.4. Effect of Catalysts 57

4.4.1. Effect of FeSO4 58

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4.4.2. Effect of CuSO4 62

4.4.3. Effect of H2O2 65

4.5. Effect of Powdered Activated Carbon (PAC) 68

4.5.1. Effect of FeSO4/PAC/US system 71

4.5.2. Effect of CuSO4/PAC /US system 74

4.5.3. Effect of H2O2/PAC/US system 76

4.6. Effect of Other and Combined Treatment Methods 77

4.6.1. Effect of Ultraviolet (UV), US/UV, UV/PAC

and UV/PAC/US system 78

4.7. Comparison of ultrasonic power density at different industrial

Wastewater 79

4.7.1. Effect of Ultrasonic Bath and Ultrasonic Bath/PAC system 81

4.8. Comparison between Malaysian Standard, Raw Landfill Leachate,

Ultrasonic Irradaition only and PAC/US system 84

4.9. Example of Cost Estimation from the installation of Ultrasound 84

5. CONCLUSION AND RECOMMENDATIONS FOR 86

FUTURE RESEARCH

5.1. Findings of Study 86

5.2. Recommendation for Future Research 88

REFERENCES 90

APPENDICES 99

BIODATA OF STUDENT 170

LIST OF PUBLICATIONS 171