要在2050年實現淨零碳排放，碳捕捉是一項必要的技術。目前最成熟的碳捕捉技術是利用胺進行的化學吸收，但仍然有許多的進步空間。在整個吸收的過程中，胺的特性是決定吸收塔設計和效率的主要因素。而最重要的特性是CO2的吸收能力和CO2的質傳速率。CO2捕獲過程中最廣泛使用的胺是乙醇胺(MEA)，其具有良好的反應速率，但吸收能力的性能有待提高。受阻胺具有巨大的吸收能力和良好的反應速率，具有巨大的潛力。受阻胺的大結構使得胺與CO2反應形成的氨基甲酸酯不穩定並水解形成碳酸氫鹽。因此，它具有良好的反應速率和較好的吸收能力。在這項工作中，我們的目標是量化空間位阻對二氧化碳吸收能力的影響，並更好地理解受阻胺的設計。平衡時 CO2 在胺水溶液中的溶解度是在高壓反應器中、在各種 CO2 負載量和溫度下測量的。本工作測量了10種胺的CO2平衡線，計算了特定條件下的CO2吸收能力，並試圖找出不同程度的阻礙對這些胺的吸收能力的影響。該相關性可用於預測給定胺結構的吸收能力。這項工作的成果將為吸收劑的選擇提供更多見解，並有助於實現淨零碳排放。

To achieve net zero carbon emissions by 2050, carbon capture is a necessary technology. The most mature technology for carbon capture is chemical absorption using amines, but there is still much room for improvement. Throughout the absorption process, the characteristics of the amine are a major factor in determining the design and efficiency of the absorption tower. The most important characteristics are CO2 absorption capacity and CO2 mass transfer rate. The most widely used amine for CO2 capture process is ethanolamine (MEA), which has a good reaction rate, but the performance in absorption capacity can be enhanced. Hindered amines have great potential because of the great absorption capacity and decent reaction rate. The large structure of hindered amine makes the carbamate which formed by the reaction of amine with CO2 unstable and hydrolyze to form bicarbonate. Therefore, it has good reaction rate and better absorption capacity. In this work, we aim to quantify the effect of steric hindrance on CO2 absorption capacity and give better understanding to design of hindered amines. The CO2 solubility in aqueous amine solution at equilibrium is measured in a high-pressure reactor in a wide range of CO2 loadings and temperatures. This work measured the CO2 equilibrium lines of 10 amines and calculated the CO2 absorption capacity under specific conditions and tried to find out the effect of different degrees of hindrance on the absorption capacity of these amines. The correlation can be used to predict the absorption capacity with given amine structures. The outcomes of this work will give more insights to absorbent selection and contribute to achieving net-zero emissions.

摘要 i
Abstract ii
LIST OF FIGURES vi
LIST OF TABLES x
Chapter 2 Introduction 1
2-1 Amine based CO2 capture 1
2-2 Solvent Selection 2
2-3 Theoretical review 3
2-3-1 CO2 Loading 3
2-3-2 Cyclic Capacity 4
2-3-3 Types of Amines 5
2-3-4 Reaction of Amines with CO2 6
2-4 Previous Studies on CO2 Absorption Capacity 8
2-5 Motivation 10
2-6 Research Scope 13
Chapter 3 Experimental Methods 14
3-1 Review of CO2 Solubility Measurement 14
3-2 Chemicals 15
3-3 Solution Preparation 17
3-4 Total Pressure Apparatus 18
3-5 Sampling Method by GC 22
3-6 Total Inorganic Carbon (TIC) 24
3-7 Titration 26
3-8 Empirical model 26
3-9 Heat of absorption 27
3-10 Simplified stoichiometric model (SSM) 27
Chapter 4 Result and Conclusion 32
4-1 Benchmark - CO2 solubility in 7m MEA solution 32
4-2 CO2 solubility in 7m MPA solution 38
4-3 CO2 solubility in 7m MIPA solution 41
4-4 CO2 solubility in 7m 2AP solution 45
4-5 CO2 solubility in 7m 2AB solution 49
4-6 CO2 solubility in 7m AMP solution 53
4-7 CO2 solubility in 7m EAE solution 57
4-8 CO2 solubility in 7m IPAE solution 61
4-9 CO2 solubility in 7m TBAE solution 65
4-10 CO2 solubility in 7m 3DMA1P solution 69
4-11 Comparison of cyclic capacity 73
4-12 Heat of absorption 76
4-13 SSM model, K1, and K2 comparison 77
Chapter 5 Conclusions 87
APPENDIX B 90
APPENDIX C 92
APPENDIX D 94
Reference 96

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