請用此 Handle URI 來引用此文件：
http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/101521完整後設資料紀錄
| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 駱尚廉 | zh_TW |
| dc.contributor.advisor | Shang-Lien Lo | en |
| dc.contributor.author | Thembeka Mabaso | zh_TW |
| dc.contributor.author | Thembeka Mabaso | en |
| dc.date.accessioned | 2026-02-04T16:27:05Z | - |
| dc.date.available | 2026-02-05 | - |
| dc.date.copyright | 2026-02-04 | - |
| dc.date.issued | 2025 | - |
| dc.date.submitted | 2026-01-21 | - |
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/101521 | - |
| dc.description.abstract | 酸性礦業排水（AMD）因其高酸度與重金屬濃度而持續受到注目。本研究以循環利用為核心，將廢竹筷再利用，製備為具高附加價值的生物炭，用於處理AMD。本研究透過傳統與微波輔助熱解兩種方式製備 11 種生物炭，並利用 BET、CHN/O、SEM-EDS、FTIR 與 XRD 進行材料孔隙結構及表面性質分析。其中以 450 W 微波熱解製得的生物炭在 Pb(II) 吸附上展現最佳效果，在吸附劑用量為2-g L-1、初始濃度50 mg L-1 的條件下達到可於24小時內達到濃度平衡，其去除率可達99.9%。吸附行為符合 Langmuir 等溫模式（qm 可達 89 mg g-1；R2 = 0.98），動力學則符合準二階反應（R2 = 1.00），顯示化學吸附為主要機制，其表面配位與靜電作用亦有相似結論。
此外，450 W 生物炭進一步以 CaCO3 與 CaCO3/TiO2 進行改質，形成 BC-CaCO3 與 BC-CaCO3/TiO2，並以 Box-Behnken RSM 設計對三種吸附劑進行最佳化。結果顯示投藥量、pH與接觸時間為關鍵因子，其BC、BC-CaCO3及BC-CaCO3/TiO2對Pb(II) 最大去除率分別為：40.65%、86.01%、74.83%，模型擬合相似度高（R2 > 0.98）。MLP 模型亦以良好準確性（R2 可達 0.997）驗證其預測結果。最佳化過程中，各生物炭的吸附均符合 Langmuir 模式，而動力學則呈現差異：BC 符合 Elovich 模式，而改質生物炭符合準二階反應，顯示化學吸附、表面不均質性、陽離子交換、碳酸鹽共沉澱以及 TiO2 強化鍵結等多重機制共同發生。熱力學分析結果證實所有最佳化系統的吸附過程皆具自發性、可行性且為放熱反應。應用於實際AMD時，BC-CaCO3/TiO2 對所有目標金屬均展現良好去除效率，在24小時內達到 97.15–99.99% 的去除率，依據其效益排序分別為為 Fe(III) > Zn(II) > Cu(II) > Mn(II) > Pb(II)，證實其適用於複雜 AMD 水質。 進一步的研究將 BC-CaCO3/TiO2 應用於人工濕地系統，包括控制組（C-CW）、僅含生物炭的人工濕地（BC-CW）以及結合生物炭與植物的人工濕地（BC/T-CW）。其中，BC-CW 改善pH 穩定性並提升 Cu、Pb 與 Zn 的固定能力，而 BC/T-CW 則展現最可靠的整體改良效果，包含維持良好氧化還原條件及更強的 Fe 與 Mn 固定能力。總體基因定序結果顯示，BC/T-CW 可促進具有植物關聯性的微生物群，並富含污染物降解相關的菌群與功能途徑，突顯工程化生物炭與香蒲（Typha latifolia）結合後在 AMD 濕地處理中的疊加效益。 總而言之，本研究證明當廢棄物來源的生物炭經過合理設計與改質，再結合生物系統後，可提供一種務實且具韌性的 AMD 處理方式。透過材料分析、吸附測試、統計最佳化、實際 AMD 驗證及人工濕地應用等整合結果皆顯示，BC-CaCO3/TiO2 無論作為單獨吸附劑或濕地系統中的原料之一時，均展現最穩定且最優越的效能。本研究強調工程材料與人工濕地生態結合，可提供一種具成本效益、循環再利用且效果良好的解決方案，用於處理富含金屬的酸性水體。 | zh_TW |
| dc.description.abstract | Acid mine drainage (AMD) remains a major concern due to its acidity and heavy metal load, and this work explores a circular approach that repurposes waste bamboo chopsticks into high-value biochars for its treatment. Eleven biochars were produced through both conventional and microwave-assisted pyrolysis and characterised using BET, CHN/O, SEM–EDS, FTIR and XRD to understand their structural and surface properties. Among these, the microwave-derived biochar produced at 450 W consistently showed the strongest Pb(II) adsorption, reaching 99.9% removal at a dose of 2 g L-1 and 50 mg L-1 initial concentration, with equilibrium achieved within 24 hours. The adsorption process followed Langmuir behaviour (qm up to 89 mg g⁻¹; R2 = 0.98) and matched pseudo-second-order kinetics (R2 = 1.00), confirming chemisorption as the primary mechanism which is supported by surface complexation and electrostatic interaction.
Furthermore, the BC produced at 450 W was further modified with CaCO3 and CaCO3/TiO2 to form BC-CaCO3 and BC-CaCO3/TiO2, and all three adsorbents were optimised using a Box–Behnken RSM design. Dose, pH and contact time emerged as key factors, yielding maximum Pb(II) removals of 40.65% for BC, 86.01% for BC-CaCO3 and 74.83% for BC-CaCO3/TiO2, with strong model fits (R2 > 0.98). MLP modelling confirmed these predictions with high accuracy (R2 up to 0.997). During optimisation, adsorption fitted the Langmuir model across all biochar, while kinetics differed; ranging from Elovich behaviour for BC and pseudo-second-order kinetics for both modified biochar which highlighted a combination of chemisorption, surface heterogeneity, cation exchange, carbonate-assisted precipitation and TiO2-enhanced binding. Thermodynamic results showed that adsorption across all optimised systems was spontaneous, favourable and endothermic. When applied to real AMD, BC-CaCO3/TiO2 demonstrated high removal of all targeted metals, achieving 97.15 - 99.99% extraction within 24 h, with a trend of Fe(III) > Zn(II) > Cu(II) > Mn(II) > Pb(II), confirming its suitability for complex AMD matrices. BC-CaCO3/TiO2, was subsequently applied to further studies which involved constructed wetlands. These wetlands included a control system (C-CW), a biochar-only wetland (BC-CW) and a combined biochar–plant wetland (BC/T-CW). While BC-CW improved pH stability and enhanced Cu, Pb and Zn retention, the BC/T-CW system delivered the most reliable improvements, maintaining favourable redox conditions and stronger Fe and Mn immobilisation. Metagenomic analysis further demonstrated that BC/T-CW supported a specialised, plant-associated microbial community enriched in pollutant-degrading taxa and functional pathways, highlighting the synergistic benefits of combining engineered biochar with Typha latifolia in wetland-based AMD treatment. In essence, this work shows that waste-derived biochar, when purposefully modified and paired with a biological system, can offer a practical and robust way to address AMD. The combination of detailed material characterisation, adsorption testing, statistical optimisation, real AMD trials, and wetland-scale application demonstrated that BC-CaCO3/TiO2 consistently delivered the strongest performance, both as a standalone adsorbent and within a functioning treatment system. The study highlights how combining engineered materials with wetland ecology can provide an affordable, circular and effective approach for mitigating metal-rich acidic waters. | en |
| dc.description.provenance | Submitted by admin ntu (admin@lib.ntu.edu.tw) on 2026-02-04T16:27:05Z No. of bitstreams: 0 | en |
| dc.description.provenance | Made available in DSpace on 2026-02-04T16:27:05Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | Doctoral Dissertation Acceptance Certificate ii
Acknowledgements iii Dedication v 摘要 vi Abstract viii Table of Contents x List of Figures xiv List of Tables xviii List of Abbreviations and Acronyms xxi Declaration of Publications xxiii Chapter 1. Introduction 1 1.1 Rationale of the Study 1 1.2 Research Aim and Objectives 2 Chapter 2. Literature Review 4 Overview 4 2.1 Introduction 5 2.2 Methods of Remediating AMD 10 2.3 Biochar 11 2.3.1 Biomass for biochar production 12 2.3.2 Biochar production: conventional pyrolysis vs microwave assisted pyrolysis 13 2.3.3 Bamboo chopsticks as biomass, biochar and for application 14 2.4 Modification of biochar 15 2.4.1 Modification using CaCO3 17 2.4.2 Modification using nanotechnology 18 2.4.3 Dual or multiple modification 20 2.5 Adsorption Experimental Factors and Mathematical Modelling 22 2.5.1 Adsorption Kinetics 23 2.5.2 Adsorption Isotherms 24 2.6 Adsorption Mechanisms 26 2.7 Process and Statistical Optimisation 28 2.8 Removal of Pb (II) and other competitive heavy metals from AMD Using Constructed Wetlands 31 2.9 Summary 34 Chapter 3. Materials and Methods 35 3.1 Research Workflow 35 3.2 Comparative Assessment of Conventional and Microwave Pyrolysis Biochars for Pb(II) Removal from Synthetic Wastewater 37 3.2.1 Biomass Composition 37 3.2.2 Biochar Preparation 37 3.2.2.1 Conventional Pyrolysis 37 3.2.2.2 Microwave-Assisted Pyrolysis 38 3.2.3 Characterization of Bamboo Chopstick Biochar 39 3.2.4 Adsorption isotherm and kinetic studies 39 3.2.5 Statistical Analyses 41 3.3. Optimisation of Pb(II) Removal Using BC, BC-CaCO3 and BC-CaCO3/TiO2 Biochar via RSM and MLP, with Application to Real Acid Mine Drainage 41 3.3.1 Preparation of Adsorbents 42 3.3.2 Characterization of Adsorbents 43 3.3.3 Determination of point of zero charge 43 3.3.4 Experimental Design and Prediction for BC, BC-CaCO3, and BC-CaCO3/TiO2 Using Response Surface Methodology 44 3.3.5 Machine Learning Prediction: Multilayer Perceptron Framework 45 3.3.6 Batch Adsorption Studies 47 3.3.7 Adsorption Experiments 47 3.3.8 Acid Mine Drainage Application 48 3.3.9 Error Analysis 48 3.4 Comparison of Constructed Wetlands for Acid Mine Drainage Treatment: Control, Biochar, and Biochar-Plant Systems 49 3.4.1 Experimental setup of constructed wetland systems 49 3.4.2 Preparation of Synthetic Acid Mine Drainage and Wetland Operation 50 3.4.3. Analytical Methods 51 3.4.3.1 Water Sampling and Analysis 51 3.4.3.2 Wetland Plant and Soil Analyses 51 3.4.3.3 Biochar 52 3.4.4. Metagenomic Studies 53 3.4.5. Statistical Analysis 54 Chapter 4. Results and Discussion 55 Overview 55 4.1. Comparative Assessment of Conventional and Microwave Pyrolysis Biochars for Pb(II) Removal from Synthetic Wastewater 56 4.1.1 Characterization of the Biochars Produced 56 4.1.1.1 Proximate Analysis 56 4.1.1.2 Temperature Profiling of Microwave-Assisted Pyrolyzed Biochar 57 4.1.1.3 Elemental Analysis 58 4.1.1.4 Surface Area and Pore Analysis 62 4.1.1.5 SEM Surface Analysis 63 4.1.1.6 FTIR of the Biochar Before Batch Adsorption 64 4.1.2 Evaluation of Batch Adsorption 66 4.1.2.1 Effect of the adsorbent dose 66 4.1.2.2 Effect of the initial Pb(II) concentration 67 4.1.2.3 Effect of Contact Time 69 4.1.2.4 Effect of Ionic Strength 70 4.1.3 Adsorption Isotherm Models 71 4.1.4 Adsorption Kinetics Models 75 4.1.5 Adsorption Mechanism Analysis 80 4.1.6 Comparison to Other Adsorbents 82 4.2 Optimisation of Pb(II) Removal Using BC, BC-CaCO3 and BC-CaCO3/TiO2 Biochar via RSM and MLP, with Application to Real Acid Mine Drainage 84 4.2.1 Characterization outcomes of BC, BC-CaCO3, and BC-CaCO3/TiO2 composites 84 4.2.2 Point of Zero Charge (pHpzc) 89 4.2.3 RSM for Pb(II) Adsorption 92 4.2.3.1 Analysis of Variance (ANOVA) Studies 96 4.2.3.2 Three-Dimensional RSM Plots 97 4.2.3.2.1 Effect of Adsorbent Dose and Time 97 4.2.3.2.2 Effect of Adsorbent Dose and pH 98 4.2.3.2.3 Effect of pH and Time 98 4.2.3.2.4 RSM Evaluation and Verification of Optimised Models 98 4.2.4 Optimisation Using Machine Learning Prediction: MLP Framework 99 4.2.5 Effect of Adsorbent Dose 106 4.2.6 Effect of pH 107 4.2.7 Adsorption Isotherm Studies 108 4.2.8 Adsorption Kinetic Studies 112 4.2.9 Thermodynamics 115 4.2.10 Adsorption Mechanism 118 4.2.11 Real Acid Mine Drainage Application Findings 124 4.3 Comparison of Constructed Wetlands for Acid Mine Drainage Treatment: Control, Biochar, and Biochar-Plant Systems 127 4.3.1 Operational Performance of CW: pH, Redox Potential and Temperature 127 4.3.2 Biochar, Plant and Soil Analysis 128 4.3.2.1 Analysis of Biochar 128 4.3.2.2 Plant and Soil Analysis 131 4.3.2.3. Bioaccumulation and Translocation Behaviour under BC/T-CW Treatment 138 4.3.3 Effect of pH on the treatment of synthetic AMD 141 4.3.4 Metagenomics 144 Chapter 5. Conclusion and Recommendations 148 5.1 Conclusion 148 5.2 Recommendations for Future Studies 150 References 152 Appendix 182 | - |
| dc.language.iso | en | - |
| dc.subject | 酸性礦業排水（AMD） | - |
| dc.subject | 竹筷生物炭 | - |
| dc.subject | 微波輔助熱解 （MAP） | - |
| dc.subject | 碳酸鈣 （CaCO3） | - |
| dc.subject | 二氧化鈦（TiO2） | - |
| dc.subject | 反應曲面法（RSM） | - |
| dc.subject | 多層感知器（MLP） | - |
| dc.subject | 人工濕地 | - |
| dc.subject | AMD | - |
| dc.subject | Bamboo Chopsticks Biochar | - |
| dc.subject | Microwave-assisted pyrolysis (MAP) | - |
| dc.subject | CaCO3 | - |
| dc.subject | TiO2 | - |
| dc.subject | Response surface methodology (RSM) | - |
| dc.subject | Multilayer perceptron (MLP) | - |
| dc.subject | Constructed wetlands | - |
| dc.title | 以蛋殼-TiO2 改質的永續竹筷生物炭用於酸礦排水中 Pb(II) 與多金屬去除之綜合解決方案 | zh_TW |
| dc.title | Sustainable Bamboo Chopstick Biochar Solutions for Pb(II) and Multi-Metal Removal from Acid Mine Drainage using Eggshell-TiO2 Modification | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 114-1 | - |
| dc.description.degree | 博士 | - |
| dc.contributor.oralexamcommittee | 林逸彬;童心欣;林耀東;胡景堯 | zh_TW |
| dc.contributor.oralexamcommittee | Yi-Pin Lin;Hsin-Hsin Tung;Yao-Tung Lin;Ching-Yao Hu | en |
| dc.subject.keyword | 酸性礦業排水（AMD）,竹筷生物炭微波輔助熱解 （MAP）碳酸鈣 （CaCO3）二氧化鈦（TiO2）反應曲面法（RSM）多層感知器（MLP）人工濕地 | zh_TW |
| dc.subject.keyword | AMD,Bamboo Chopsticks BiocharMicrowave-assisted pyrolysis (MAP)CaCO3TiO2Response surface methodology (RSM)Multilayer perceptron (MLP)Constructed wetlands | en |
| dc.relation.page | 186 | - |
| dc.identifier.doi | 10.6342/NTU202600121 | - |
| dc.rights.note | 同意授權(全球公開) | - |
| dc.date.accepted | 2026-01-22 | - |
| dc.contributor.author-college | 工學院 | - |
| dc.contributor.author-dept | 環境工程學研究所 | - |
| dc.date.embargo-lift | 2026-02-05 | - |
| 顯示於系所單位： | 環境工程學研究所 | |
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