應用PVA/PG/SBA-15混合基質薄膜提升二氧化碳分離性能之評估研究

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常明文(Truong Minh Man) 查詢紙本館藏

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應用PVA/PG/SBA-15混合基質薄膜提升二氧化碳分離性能之評估研究
(Enhanced CO2 separation performance by PVA/PG/SBA-15 mixed matrix membranes)

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至系統瀏覽論文 (2029-8-19以後開放)

摘要(中)

本研究使用中孔SiO2製備平均孔徑為3.13 nm的球形分子篩 (Santa Barbara Amorphous-15, SBA-15) 做為薄膜之基質，並添加含有聚乙烯醇 (polyvinyl alcohol, PVA) 及甘胺酸哌? (piperazine glycinate, PG) 的溶液，以製備混合基質薄膜 (mixed matrix membranes, MMMs) ，並針對製備之薄膜進行材料特性及氣體分離試驗分析。透過FT-IR 光譜測試，在波數為 1,144 cm-1 時，發現縮醛形成的交聯結構；以及在波數為 1,060 cm-1 時，觀察到Si-O-Si 伸縮振動及彎曲振動的特徵峰，並在 1,610 cm-1 處偵測到N-H 官能基的峰值。藉由增加 SBA-15 的濃度，可以提升薄膜的機械強度及熱穩定性，以及擴大非晶形區域，且因基質與CO2具有高相容性，能提升對CO2的穿透率及選擇性。隨著SBA-15 載量的增加，可使其在薄膜上分布更加均勻，然而，顆粒聚集現象亦逐漸顯著發生。氣體分離之試驗結果顯示，含有 15 wt.% SBA-15 的薄膜 PVA/PG/SBA-15，可達到711.6 Barrer的最佳 CO2 穿透率及150.75的CO2/N2 選擇性，明顯優於2008 年 Robeson之研究成果。由於 MMMs 中PG的胺基存在， CO2 得依溶滲機制進行分離。整體而言，本研究製備之MMMs 具有優異的氣體分離效果，特別是應用於分離 CO2、淨化氣體及控制 CO2 排放等方面，未來極具工業應用分離氣體之發展潛力。

摘要(英)

This study investigates the addition of spherical mesoporous silica SiO2 Santa Barbara Amorphous-15 (SBA-15), with an average pore size of 3.13 nm, into a solution containing polyvinyl alcohol (PVA) and piperazine glycinate (PG). Characteristic investigations and gas separation tests were conducted on the MMMs. The FTIR spectra confirmed the acetal structures formed by cross-linking at a wavenumber of 1144 cm-1 and the Si-O-Si stretching and bending bond at a wavenumber of 1060 cm-1. Moreover, the peak detected at 1610 cm-1 suggested the presence of the N-H group in the PVA/PG/SBA-15 membrane. Increasing the concentration of SBA-15 resulted in the enhancement of mechanical and thermal performances of the membrane, as well as an increase in the amorphous region. The rise in CO2 permeability and selectivity resulted from the high compatibility and addition of mobile carriers. As SBA-15 loading increased, the dispersion of the filler improved, but there was also a noticeable increase in particle agglomeration. The findings showed that the PVA/PG membrane, with a 15 wt.% of SBA-15 loading PVA/PG/SBA-15, had both the optimal CO2 permeability of 711.6 Barrer and CO2/N2 selectivity of 150.75. These values were placed beyond 2008 Robeson’s upper bound. The solution-diffusion mechanism dominates CO2 separation due to the presence of amine groups from PG in the MMMs. The excellent gas separation performance of the prepared MMMs has a good potential for industrial gas separation, particularly in separating CO2, purifying gases, and controlling CO2 emissions.

關鍵字(中)

★ 無機填料
★ 中孔二氧化矽
★ 球形SBA-15
★ 混合基質薄膜
★ 二氧化碳分離
★ 聚乙烯醇

關鍵字(英)

★ Inorganic filler
★ mesoporous silica
★ spherical SBA-15
★ mixed matrix membrane
★ carbon dioxide separation
★ polyvinyl alcohol

論文目次

摘要 i
Abstract iii
Acknowledgment iv
Table of Contents v
List of Figures ix
List of Tables xi
Chapter 1 Introduction 1
Chapter 2 Literature Review 7
2.1 Current CO2 separation technologies 7
2.2 Types of membranes used for separation 12
2.2.1 Polymeric membranes 12
2.2.2 Inorganic membranes 16
2.2.3 Mixed-matrix membranes (MMMs) 17
2.3 Potential fillers for Mixed Matrix Membranes 22
2.3.1 Mesoporous silica SBA-15 23
2.3.2 Zeolites 24
2.3.3 Graphene (GO) 25
2.3.4 Carbon nanotubes 26
2.3.5 Metal-organic framework (MOF) 26
2.4. Transport theory for gas membrane separation 28
2.4.1 Gas transport mechanisms in porous membranes 28
2.4.2 Gas transport mechanisms in dense (non-porous) membranes 29
2.4.3 Limitations of polymeric membranes 33
2.5 Membrane fabrication techniques 34
2.5.1 Solution casting technique 34
2.5.2 Phase-Inversion technique 34
2.5.3 Dip-coating technique 35
2.5.4 Spin-coating technique 35
2.6 Influential factors on the structure and MMMs performance 38
2.6.1 Crystallinity and glass transition temperature 38
2.6.2 Free volume 39
2.6.3 Swelling 40
2.6.4 Crosslinking 41
2.6.5 Choice of filler and polymer 42
2.6.6 Filler dispersion 42
2.6.7 Filler and polymer interfacial interaction 44
2.6.8 Plasticization and physical aging 45
2.7 Modification methods for MMMs 47
2.7.1 Filler size, shape and loading modification. 48
2.7.2 Adding additives to MMMs. 49
2.7.3 Filler surface adjustment 52
2.7.4 In-situ synthesis of MMM 52
2.8 Design thinking for the research proposal 53
Chapter 3 Materials and Methods 55
3.1 Materials 55
3.2 Membrane preparation 55
3.2.1 Synthesis of piperazine glycinate salt 55
3.2.2 Synthesis of spherical SBA-15 56
3.2.3 Synthesis of PVA/PG and PVA/PG/SBA-15 57
3.2.4 CO2/N2 gas permeation test 59
3.3 Characterization of spherical SBA-15 filler and MMMs 61
3.3.1 Filler characterization 61
3.3.2 Membrane characterization 62
Chapter 4 Results and Discussion 63
4.1 Characterization of SBA-15 fillers 63
4.1.1 Thermal properties of SBA-15 fillers 63
4.1.2 Chemical properties of SBA-15 fillers 64
4.1.3 Morphological and structural properties of SBA-15 fillers 66
4.1.4 Textural properties of SBA-15 fillers 67
4.2 Characterization of MMMs 69
4.2.1 Chemical properties of MMMs 69
4.2.2 Morphologies properties of MMMs 70
4.2.3 Structural properties of MMMs 72
4.2.4 Thermal properties of MMMs 73
4.2.5 Mechanical properties of MMMs 74
4.3 Membrane separation performance 75
4.3.1 The effect of SBA-15 loading on CO2/N2 separation of PVA/PG/SBA-15 MMMs 75
4.3.2 Comparison of PVA/PG/SBA-15 MMMs with previous research 79
4.4 Proposed mechanisms of MMMs 81
Chapter 5 Conclusions and Recommendations 83
5.1 Conclusions 83
5.2 Recommendations 84
Bibliography 87
Appendix 105

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指導教授

江康鈺(Kung-Yuh Chiang)

審核日期

2024-8-19

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