臺灣博碩士論文加值系統

隨著薄膜電晶體液晶顯示器與半導體產業的發展，生產過程廣泛使用的化學藥品也隨之增加。其中，氫氧化四甲銨(Tetramethylammonium hydroxide, TMAH) 是發光二極體生產使用顯影劑的主要成分，同時也運用於半導體製造中的鹼性蝕刻液和清洗液。由於含有氫氧化四甲銨的廢水溶液具有強鹼性與劇毒性，因此排放前必須妥善處理。
本研究利用商業化離子交換樹脂進行離子交換程序，並探討強酸與弱酸兩種陽離子交換樹脂對於氫氧化四甲銨溶液的去除效能。研究結果顯示，強酸陽離子樹脂與弱酸陽離子交換樹脂分別進行離子交換程序20分鐘與40分鐘後即可達到平衡。並將實驗數據利用Pseudo二階動力學方程式表示，相較於弱酸陽離子交換樹脂，強酸陽離子交換樹脂具有較快的交換速率。在研究溶液pH的影響中，當溶液平衡pH值維持高於6.5時，發現影響較大的為弱酸陽離子交換樹脂。利用Freundlich和Langmuir吸附等溫曲線計算，結果顯示吸附作用是合適的，根據Langmuir參數，弱酸陽離子交換樹脂與TMA+具有較強的交互作用。經過鹽酸進行脱附作用後，顯示本研究使用之離子交換樹脂進行五個循環程序後仍然維持良好去除效能。計算TMA+吸附的選擇系數，分別得到強酸陽離子交換樹脂為5.16，弱酸陽離子交換樹脂為46.28。
由於溶液中的干擾離子會影響TMA+的吸附，因此，本研究進而探討不同離子對於TMA+進行離子交換程序過程中的吸附影響。結果發現，由於胺分子與離子交換樹脂之間的強交互作用，因此TMA+的吸附程度下降37%。

Due to the rise in thin-film transistor liquid crystal display and semiconductor manufacturing, amount of chemicals extensively used in production process have increased as well. Tetramethylammonium hydroxide (TMAH) is one the chemicals, widely used as a major ingredient of photoresist developer in light emitting diode (LED) production, as well as an alkaline etchant and cleaning solution in semiconductor manufacturing. TMAH is a strong base and highly toxic, thus TMAH-containing wastewater has to be properly treated before it is discharged to the environment.
In this study, ion exchange process using commercial ion exchange resin was selected. Two cation exchange resins, namely strong acid (SAC) and weak acid (WAC) cation exchange resin were used to remove TMAH from aqueous solution. Both resins showed high TMA+ ion removal. Ion exchange process was completed within 20 minutes when using SAC and 40 minutes when using WAC. Pseudo second order kinetics model was chosen to represent experimental data, which showed that SAC has faster exchange rate compared to WAC. Investigation on the effect of solution pH revealed WAC was more predominantly affected, and equilibrium pH above 6.5 needs to be maintained. Freundlich and Langmuir adsorption isotherm showed that adsorption was favorable; with Langmuir parameters implied that WAC has stronger interaction with TMA+ compared to SAC. Desorption study using HCl suggested that ion exchange resins used in this study can performed well after 5 cycles. Calculated selectivity coefficient for TMA+ uptake using SAC and WAC was 5.16 and 46.28, respectively.
The presence of interfering ions, both simple and more complex ones, affected TMA+ uptake. When amines were present in solution, the extent of TMA+ uptake decrease was as high as 37%, due to strong interaction between resin matrix with amine molecule

CONTENTS

ABSTRACT i
ABSTRACT (in Chinese) ii
ACKNOWLEDGEMENTS iii
NOMENCLATURES iv
CONTENTS v
LIST OF FIGURES vii
LIST OF TABLES viii
CHAPTER 1. INTRODUCTION 1-1
1.1. Background 1-1
1.2. Objective 1-2
1.3. Scope of research 1-2
CHAPTER 2. LITERATURE REVIEW 2-1
2.1. Tetramethylammonium hydroxide (TMAH) 2-1
2.2. Treatment of TMAH-containing wastewater 2-2
2.3. Ion exchange 2-7
2.4. Ion exchangers 2-8
2.5. Kinetics 2-10
2.6. Ion exchange equilibrium 2-11
2.6.1. Adsorption isotherms 2-11
2.6.2. Selectivity coefficient 2-12
2.7. The effect of interfering ions on ion exchange 2-13
2.8. Basicity of amines 2-15
CHAPTER 3. MATERIALS AND METHODS 3-1
3.1. Materials 3-1
3.2. Instruments 3-2
3.3. Experimental designs and methods 3-2
3.3.1. Resin preparation 3-3
3.3.2. Surface area measurement of WAC 3-4
3.3.3. Ion exchange of TMAH 3-5
3.3.3.1. Adsorption isotherm 3-6
3.3.3.2. Kinetic study 3-6
3.3.3.3. Effect of pH 3-7
3.3.3.4. Regeneration study 3-8
3.3.3.5. Selectivity coefficient determination (SAC and WAC) 3-9
3.3.3.6. Selectivity coefficient determination (interfering ions) 3-9
3.3.3.7. Effect of interfering ions on TMA+ uptake 3-10
3.4. Ab-initio proton affinity calculation 3-10
3.4.1. Information on GaussView 5.0 3-11
3.4.2. Gaussian command 3-11
CHAPTER 4. RESULTS AND DISCUSSION 4-1
4.1. Resin characterization - SEM 4-1
4.2. Equilibrium time determination of TMA+ uptake using cation exchange resin 4-2
4.3. Effect of resin dose on TMA+ uptake 4-4
4.4. Adsorption isotherms of TMA+ uptake 4-6
4.5. Reaction kinetics of TMA+ uptake 4-9
4.6. Desorption study 4-12
4.7. Ion exchange modeling 4-16
4.7.1. SAC 4-17
4.7.2. WAC 4-18
4.8. Effect of interfering ions on TMA+ uptake using SAC 4-22
4.8.1. Ammonium, potassium, magnesium, sodium 4-22
4.6.2. Primary, secondary, tertiary amines 4-30
4.9. Discussion

CHAPTER 5. CONCLUSIONS AND RECOMMENDATIONS 5-1
5.1. Conclusions 5-1
5.2. Recommendations 5-2
REFERENCES R-1
APPENDIX A : EXPERIMENTAL DATA A-1
APPENDIX B: GAUSSIAN OUTPUT B-1

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