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http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/101727完整後設資料紀錄
| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 郭大孚 | zh_TW |
| dc.contributor.advisor | Ta Fu Dave Kuo | en |
| dc.contributor.author | 黃維得 | zh_TW |
| dc.contributor.author | Wei-Te Huang | en |
| dc.date.accessioned | 2026-02-26T17:03:13Z | - |
| dc.date.available | 2026-02-27 | - |
| dc.date.copyright | 2026-02-26 | - |
| dc.date.issued | 2026 | - |
| dc.date.submitted | 2026-01-20 | - |
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/101727 | - |
| dc.description.abstract | 微塑膠（MPs）可作為有機污染物的載體，透過吸收或吸附作用影響其在環境中的分佈、毒性與生物可利用性。儘管已有大量關於有機化合物在不同微塑膠上的吸附行為之研究與實驗，但由於微塑膠與有機化合物的多樣性，以及實驗條件的差異，至今仍難以形成一致而全面的理解。
本研究旨在透過分析與建模不同微塑膠與有機化合物的實驗吸附係數，建立對有機物—微塑膠吸附行為的整體認識。我們整理了一個包含13種微塑膠與31種有機化合物的有機碳歸一化吸附係數（KOC）資料庫，共收錄3654組數據，來自83篇實驗研究。時間尺度分析顯示，約49% 的吸附數據（主要是玻璃態微塑膠）可能未達到吸附平衡。有機化合物在玻璃態微塑膠中的擴散速率極慢，擴散係數約為10-14 cm2/s，遠低於橡膠態微塑膠中的值（約10-10 cm2/s），這意味著若要達到平衡吸附，玻璃態微塑膠可能需長達一年以上的吸附時間。與天然有機質（NOM）相比，96% 的微塑膠–化合物對的log KOC小於或等於（69%等於）NOM–化合物對的log KOC，顯示NOM的分配行為可作為微塑膠吸附的上限估值。這一趨勢在不同類型的微塑膠、化合物以及可電離化合物（如四環黴素與三氯生）中皆一致。 進一步分析顯示，微塑膠的log KOC主要受化合物特性所主導，而非微塑膠本身的性質所決定。化合物的疏水性（如log KOW、極性表面積）在89%的微塑膠中與log KOC顯著相關，反之微塑膠的極性、結晶度、密度及與水接觸角等性質僅具弱或可忽略的影響。線性溶劑化能關係（LSER）模型僅能針對PE與PCL建立（RMSE:0.06–0.36），其餘微塑膠因未達平衡或資料不足而無法建模。模型中McGowan體積係數（v=2.5–2.8）在不同模型間保持穩定，顯示吸附行為主要受空腔形成作用主導，此結果與NOM–MP比較及log KOC與化合物性質的相關性結果一致。 整體而言，本研究指出微塑膠的化學組成在有機化合物吸附中僅扮演次要角色，而NOM的分配行為可作為評估微塑膠污染水環境中有機污染物遷移性與可利用性之實用上限參考，無需區分微塑膠種類。未來仍需進一步探討化合物種態與電離行為對微塑膠log KOC的影響，以及玻璃態、擴散受限微塑膠中化合物的結合機制。 | zh_TW |
| dc.description.abstract | Microplastics (MPs) can serve as carriers of organic pollutants and influence their distribution, toxicity, and bioavailability in the environment through absorption or adsorption. Although the sorption of organic chemicals to different MPs has been extensively studied and experimented, the diverse nature of MPs and organic chemicals and varying experimental conditions have prevented a coherent understanding of the phenomenon from emerging. This study aims to develop a holistic understanding of organic-MP binding by analyzing and modeling experimental sorption coefficients of different MPs and organic sorbates. A sorption database of organic-carbon normalized sorption coefficient (KOC) (n=3654) encompassing 13 MPs and 31 organic chemicals is curated from 83 primary experimental studies. Timescale analysis reveals that 49% of the sorption data, mostly associated with glassy MPs, likely has not reached chemical equilibrium. Organic sorbates diffuse through glassy MPs very slowly with diffusivities in the order of 10-14 cm2/s, which are orders of magnitude lower than those in rubbery MPs (~10-10 cm2/s). This implies that a yearly incubation time is needed to achieve sorption equilibrium with glassy MPs. When compared against natural organic matter (NOM), 96% of MPs-sorbate pairs have log KOC less than or equal (69%) to those of NOM-sorbate pairs, suggesting NOM partitioning may serve as an upper estimate of log KOC in MPs. This is observed across MPs, chemicals, and ionizable compounds (tetracycline and triclosan). Analysis reveals that log KOC of MPs is dominated by chemical properties rather than MP properties. Chemical hydrophobicity (e.g., log KOW, polar surface area) significantly correlate with log KOC in 89% of MPs, whereas MP properties (polarity, crystallinity, density, and water contact angle) have weak or negligible influence. Linear solvation energy relation (LSER) models (RMSE: 0.06–0.36) are constructed only for PE and PCL; the remaining MPs cannot be modeled due to non-equilibrium or insufficient data. The McGowan volume coefficient remains conserved across models (v=2.5–2.8), suggesting sorbate-MP association is dominated by cavity formation, which is consistent results from NOM-MP comparison and log KOC and sorbate properties correlation. Overall, this study suggests that MP chemistry plays a secondary role in the sorption of organic chemicals. Furthermore, NOM partitioning may serve as a practical upper bound reference for assessing mobility and available of organic pollutants in MP-contaminated aquatic environments without the need to differentiate plastic type. Further investigations are needed to clarify the role of speciation/ionization on log KOC of MPs and the binding of chemicals with glassy diffusion-limited MPs. | en |
| dc.description.provenance | Submitted by admin ntu (admin@lib.ntu.edu.tw) on 2026-02-26T17:03:13Z No. of bitstreams: 0 | en |
| dc.description.provenance | Made available in DSpace on 2026-02-26T17:03:13Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | 致謝 i
摘要 ii Abstract iv Contents vi List of Figures x List of Tables xii Chapter 1 Introduction 1 1.1 Background 1 1.2 Research Objectives 3 Chapter 2 Literature Review 4 2.1 Generation, Sources, and Environmental Distribution of Microplastics 4 2.2 Environmental Roles of Microplastics on Sorption of Organic Pollutants 7 2.3 Influence of Physical Properties of Microplastics on Sorption Capacity 9 2.4 Mechanism of Organic Pollutant Sorption by Microplastics 10 2.5 Comparison of Chemical Structures between Natural Organic Matter and MPs 12 2.6 Predictive Models for Microplastic Sorption Capacity 13 Chapter 3 Materials and Method 15 3.1 Search of Microplastics Sorption Data 15 3.2 Microplastics Sorption Data Compilation 16 3.3 Data Processing 28 3.3.1 Calculation of Sorption Capacities 28 3.3.2 Calculation of Ionic Species Fraction 29 3.3.3 Estimation of Ion State Sorption Coefficients 31 3.3.4 Standardize Microplastic Particle Size 32 3.4 Error in Sorption Data 33 3.4.1 Logarithmic Transformation of Variability Indicators 33 3.4.2 Propagated and Experimental Error in Sorption Data 34 3.5 Data Screening Based on Sorption Experiment Quality 35 3.5.1 The Diffusion Coefficient and Equilibrium Time of the Chemical in MPs 35 3.5.2 Use of Plastic Containers in Sorption Experiments 40 3.5.3 Inconsistencies Between Reported Sorption Parameters and Figures/Tables 41 3.5.4 Aqueous Concentrations Exceeding Initial Concentrations or Solubility 42 3.5.5 Mass Imbalance of Solutes Before and After Sorption 43 3.5.6 Sorption Data with Extremely High or Low Freely Dissoled Fraction 45 3.6 Collection of Sorption Data for Natural Organic Matter 47 3.6.1 Compilation and Processing of Natural Organic Matter Sorption Data 47 3.7 Model Establishment Process 49 3.7.1 Overall Model Development Framework 49 3.7.2 Development of LSER Models for Microplastics 50 Chapter 4 Results and Discussion 52 4.1 Data Overview and Quality Control 52 4.1.1 Selection of Chemicals and Microplastics in the Database 52 4.1.2 Summary of Experimental Conditions and Reported Parameters 57 4.1.3 Most Sorption Experimental Data are Non-Equilibrium 59 4.1.4 Setting the Tolerance Error for Sorption Data 62 4.1.5 Data Excluded Due to the Use of Plastic Containers 63 4.1.6 Data Excluded Due to Inconsistent Reporting of Sorption Results 65 4.1.7 Exclusion of Data Exceeding Initial Concentration or Solubility Limits 66 4.1.8 Data Excluded Due to Mass Balance Ratio 67 4.1.9 Data Excluded Due to Freely Dissolved Fraction Values 69 4.1.10 Compilation of NOM Sorption Data and Comparative Characteristics of NOM and Microplastics 72 4.1.11 Model Dataset Used 74 4.2 Comparison of Sorption between MPs and NOM 76 4.2.1 NOM Exhibits Higher log KOC than MPs with Few Exceptions 76 4.2.2 Limited Effect of Chemical Ionization on log KOC between MPs and NOM 82 4.2.3 MPs Polarity, Tg, Pore Volume and SSA Cannot Explain the log KOC Differences between MPs and NOM 87 4.3 Factors Controlling Sorption Variability between Microplastics and Chemicals 92 4.3.1 Dominant Effects of Chemical Hydrophobicity and Polarity on log KOC 92 4.3.2 Limited Influence of Polymer Type Properties on Sorption Capacitys 100 4.3.3 SSA Has a Limited Effect on Sorption Capacity 106 4.3.4 Weak Effects of Salinity and Temperature on Sorption Capacity 108 4.4 Development and Mechanistic Interpretation of LSER Model for MPs Sorption 111 4.4.1 Development and Validation of LSER Models for Microplastics log KOC 111 4.4.2 Effect of Chemical Activity Control on Model Robustness and Accuracy 116 4.4.3 Molecular Interaction Mechanisms Revealed by LSER Coefficients 118 Chapter 5 Conclusions and Suggestion 120 5.1 Conclusions 120 5.2 Future Work 121 References 122 Appendixes 142 Appendix 1. Spreadsheet 142 Appendix 2. log KOC of MP-Chemical Pairs After Data Quality Screening 143 Appendix 3. Supplementary Information on Chemical and Property 144 Appendix 4. Collection of MP Contact Angle and pzc Experimental Values 148 Appendix 5. Characteristic Distribution and Range in Sorption Data 149 Appendix 6. Polymer Supplier Report Cross-Linked Checklist 150 Appendix 7. Effect of Using PTFE on Kd in Sorption Experiments 151 Appendix 8. Effect of chemical properties on log KOC 152 Appendix 9. Effect of With or Without Light Exposureon and Biocide on Kd 156 Appendix 10. Distribution of E, S, A, B, V Parameters in Modeling Data 159 Appendix 11. Reference 160 | - |
| dc.language.iso | en | - |
| dc.subject | 微塑膠 | - |
| dc.subject | 有機污染物 | - |
| dc.subject | 有機碳歸一化吸附係數 | - |
| dc.subject | 平衡吸附 | - |
| dc.subject | 天然有機質 | - |
| dc.subject | 線性溶劑化能關係 | - |
| dc.subject | Microplastics | - |
| dc.subject | Organic chemical | - |
| dc.subject | KOC | - |
| dc.subject | Equilibrium | - |
| dc.subject | Natural organic matter | - |
| dc.subject | LSER | - |
| dc.title | 有機化合物於微塑膠上的吸附：薈萃分析與建模 | zh_TW |
| dc.title | Sorption of Organic Chemicals to Microplastics: Meta-analysis and Modeling | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 114-1 | - |
| dc.description.degree | 碩士 | - |
| dc.contributor.oralexamcommittee | 施養信;林逸彬;吳先琪 | zh_TW |
| dc.contributor.oralexamcommittee | Yang-Hsin Shih;Yi-Pin Lin;Shian-Chee Wu | en |
| dc.subject.keyword | 微塑膠,有機污染物有機碳歸一化吸附係數平衡吸附天然有機質線性溶劑化能關係 | zh_TW |
| dc.subject.keyword | Microplastics,Organic chemicalKOCEquilibriumNatural organic matterLSER | en |
| dc.relation.page | 162 | - |
| dc.identifier.doi | 10.6342/NTU202600162 | - |
| dc.rights.note | 同意授權(限校園內公開) | - |
| dc.date.accepted | 2026-01-20 | - |
| dc.contributor.author-college | 工學院 | - |
| dc.contributor.author-dept | 環境工程學研究所 | - |
| dc.date.embargo-lift | 2028-01-19 | - |
| 顯示於系所單位： | 環境工程學研究所 | |
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