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研究生：	吳仲恩 Wu, Zhong-En
論文名稱：	冷燒結技術穩定/固化飛灰中重金屬之研究 Stabilization/Solidification of Municipal Solid Waste Incineration Fly Ash via Cold Sintering Process
指導教授：	申永輝 Shen, Yun-Hwei
學位類別：	碩士 Master
系所名稱：	工學院 - 資源工程學系 Department of Resources Engineering
論文出版年：	2022
畢業學年度：	111
語文別：	中文
論文頁數：	190
中文關鍵詞：	焚化飛灰、冷燒結技術、重金屬固化、資源化、田口方法
外文關鍵詞：	MSWI fly ash, cold sintering process, heavy metal solidification, resource utilization, Taguchi method
相關次數：	點閱：253 下載：11
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查詢本校圖書館目錄查詢臺灣博碩士論文知識加值系統勘誤回報

都市廢棄物在焚化後所產生的飛灰(MSWI FA)在近年來對於台灣這片土地的影響逐年上升。現階段採用的穩定/固化方式會導致體積大幅膨脹，需要更多的空間進行放置，且穩定/固化後的飛灰無法再進行進一步的資源化利用。飛灰當中主要由鈣、矽化合物所構成，同時還包含重金屬、氯鹽、硫酸鹽、有機污染物等複雜成分，如何有效克服這些內部有害物質帶來的影響，將是飛灰資源化最大的挑戰。本次研究重點將聚焦於冷燒結技術是否能夠有效固化飛灰當中的指標重金屬，並探討其中的運作機制。
本研究將使用城西焚化廠之焚化飛灰作為研究對象，在經過烘乾、球磨、過篩後進行XRF、王水消化、XRD、SEM、雷射粒徑、熱重分析。並利用田口式直交表進行冷燒結技術二水準、四水準之L16直交表實驗，實驗因子包含溫度、壓力、時間、液體添加比例、碳酸鈉添加比例。二水準L16直交表實驗為探討因子間交互作用情形，四水準L16直交表實驗為探討最佳冷燒結技術固化飛灰的最佳條件。實驗結果表明在溫度300℃、單軸壓力10T (312 MPa)、時間60 mins、液體(水)添加25 wt%、碳酸鈉添加9 wt%下所製備出來的飛灰塊材與飛灰原樣TCLP結果相比能夠有效減少溶出鎘(Cd) 77.71%、鉛(Pb) 21.14%、鋅(Zn)42.37%、鉻(Cr) 99.99%。
飛灰最佳條件冷燒結塊材XRD結果相較於飛灰原樣多出了鈣長石、鈉柱石、矽酸鈣、水鈣鋁榴石等二次相，並將重金屬固化於其中。SEM-EDS結果顯示部分重金屬會在冷燒結過程中受到液體由內而外蒸發影響被攜帶至塊材表面，間接導致固化效果不如預期。

To investigate the effects of various factors on the solidification of fly ash using cold sintering process, the Taguchi orthogonal array L16 design was employed to conduct two-level and four-level L16 orthogonal array experiments. The experimental factors included temperature, pressure, time, liquid-to-solid ratio, and sodium carbonate addition.

The two-level L16 orthogonal array experiment was conducted to assess the interaction between factors, while the four-level L16 orthogonal array experiment was conducted to determine the optimal conditions for solidifying fly ash using cold sintering process. The results of the experiments showed that fly ash under the conditions of a temperature of 300℃, uniaxial pressure of 10T (312 MPa), a holding time of 60 minutes, 25 wt% water addition, and 9 wt% sodium carbonate addition could effectively reduce the leaching of cadmium by 77.71%, lead by 21.14%, zinc by 42.37%, and chromium by 99.99%, as compared to the original fly ash TCLP results.

Compared to the original fly ash, the XRD results of the fly ash ceramic bulk under the optimal conditions showed the presence of secondary phases, such as anorthite, marilite , calcium silicate, and hydrogrossular. These phases effectively immobilized the heavy metals in the fly ash.

However, SEM-EDS results indicated that some heavy metals were carried to the surface of the fly ash bulk during the cold sintering process due to the evaporation of liquid from the inside out. This may have indirectly affected the solidification efficiency, which was lower than expected.

摘  要	II
Abstract	III
誌  謝	XVII
目  錄	XIX
圖目錄	XXII
表目錄	XXVI
第一章	前言	1
1-1  研究源起	1
1-2  研究動機與目的	4
第二章	文獻回顧	6
2-1  焚化飛灰的產生	6
2-1-1  焚化系統運作	6
2-1-2  飛灰種類與基本性質	8
2-1-3  飛灰處理技術	10
2-2  飛灰資源化趨勢	13
2-2-1  溶出試驗種類與溶出機制	15
2-2-2  飛灰中有害物質對於資源化之困境	21
2-3  冷燒結技術	25
2-3-1	燒結理論	26
2-3-2	超低能量燒結技術	30
2-3-3	冷燒結技術發展與應用可行性	35
2-4  田口方法	49
2-4-1  田口方法簡介	49
2-4-1-1  田口方法起源	49
2-4-1-2  田口玄一博士	49
2-4-1-3  田口方法執行步驟與重要名詞解釋	52
2-4-2	實驗設計法中直交表的應用	57
2-4-2-1	直交表介紹	57
2-4-2-2	建構實驗模式	60
2-4-3	品質損失與S/N比	65
2-4-3-1  品質損失	65
2-4-3-2  S/N比	71
第三章	研究方法與實驗流程	75
3-1  實驗架構	75
3-2  實驗材料與設備	76
3-2-1  實驗藥品列表與說明	77
3-2-2  實驗儀器設備列表與說明	78
3-3  實驗流程與方法	83
3-3-1  飛灰基本性質分析	83
3-3-2  CSP前處理	84
3-3-3  以田口方法進行飛灰CSP實驗	87
3-3-4  TCLP (toxicity characteristic leaching procedure)	90
3-3-5	驗證實驗與飛灰CSP後塊材分析	92
第四章	結果與討論	95
4-1  飛灰基本性質分析	95
4-1-1  XRF分析	95
4-1-2  王水全消化分析	96
4-1-3  XRD分析	97
4-1-4  SEM初步分析	100
4-1-5  雷射粒徑分析	102
4-1-6  熱重分析(TGA)	104
4-1-7  飛灰原樣TCLP	106
4-2  飛灰CSP前處理	107
4-3  L16(215)二水準直交表實驗	111
4-3-1  L16(215)直交表實驗結果	112
4-3-2  因子間交互作用情形與變異性分析	117
4-4  L16(45)四水準直交表實驗	127
4-5  飛灰CSP確認實驗	137
4-5-1  CSP最佳實驗參數驗證與比較	138
4-5-2  實驗模式的擴展	142
4-5-2-1  鎘(Cd)之實驗模式擴展	143
4-5-2-2  鉛(Pb)之實驗模式擴展	147
4-6  飛灰CSP後塊材分析	151
4-6-1  XRD分析	151
4-6-1-1  CSP最佳條件飛灰塊材與飛灰原樣差異	151
4-6-1-2  溫度對於飛灰CSP塊材之影響	153
4-6-1-3  壓力對於飛灰CSP塊材之影響	155
4-6-1-4  時間對於飛灰CSP塊材之影響	157
4-6-1-5  液體比對於飛灰CSP塊材之影響	159
4-6-1-6  成分(碳酸鈉添加量)對於飛灰CSP塊材之影響	161
4-6-2  SEM / EDS分析	163
4-6-2-1  飛灰CSP塊材之表面 / 斷面形貌分析	163
4-6-2-2  飛灰CSP塊材之重金屬分布分析	167
4-6-3  飛灰CSP對於內部重金屬穩定 / 固化機制綜述	171
第五章	結論與建議	174
5-1	結論	174
5-2	建議	177
Reference	179
                                    

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1. TEPA. 2007; Available from: http://www.epa.gov.tw.
2. Huang, C.-M., et al., The potential of recycling and reusing municipal solid waste incinerator ash in Taiwan. Waste Management, 2006. 26(9): p. 979-987.
3. Weichenthal, S., et al., The impact of a landfill fire on ambient air quality in the north: A case study in Iqaluit, Canada. Environmental Research, 2015. 142: p. 46-50.
4. Kamal, N.L.M., et al., Immobilization of Heavy Metals for Building Materials in the Construction Industry – an Overview. Materials Today: Proceedings, 2019. 17: p. 787-791.
5. Sajwan, K.S., T. Punshon, and J. Seaman, Production of coal combustion products and their potential uses, in Coal combustion byproducts and environmental issues. 2006, Springer. p. 3-9.
6. Kirkelund, G.M., L. Skevi, and L.M. Ottosen, Electrodialytically treated MSWI fly ash use in clay bricks. Construction and Building Materials, 2020. 254: p. 119286.
7. 行政院環保署. 垃圾焚化營運年報. 2020.
8. Lin, S.-L., et al., Ultra-low PCDD/F emissions and their particle size and mass distribution in a hazardous waste treatment system. Journal of Hazardous Materials, 2022. 423: p. 127032.
9. Ren, P., K.H. Mo, and T.-C. Ling, Chapter 10 - Stabilization/solidification of municipal solid waste incineration fly ash, in Low Carbon Stabilization and Solidification of Hazardous Wastes, D.C.W. Tsang and L. Wang, Editors. 2022, Elsevier. p. 141-156.
10. Zhang, J., et al., A novel approach for preparing glass ceramic foams from MSWI fly ash: foaming characteristics and hierarchical pore formation mechanism. Journal of Materials Research and Technology, 2022. 18: p. 731-744.
11. Fan, C., et al., A comparative study on solidification/stabilization characteristics of coal fly ash-based geopolymer and Portland cement on heavy metals in MSWI fly ash. Journal of Cleaner Production, 2021. 319: p. 128790.
12. del Valle-Zermeño, R., et al., Aggregate material formulated with MSWI bottom ash and APC fly ash for use as secondary building material. Waste Management, 2013. 33(3): p. 621-627.
13. Zhang, H.Y. Analysis of macro-performance of FA ceramic brick. in Advanced Materials Research. 2014. Trans Tech Publ.
14. Giro-Paloma, J., J. Formosa, and J.M. Chimenos, Granular material development applied in an experimental section for civil engineering purposes. Applied Sciences, 2020. 10(19): p. 6782.
15. Huang, B., et al., Recent progress on the thermal treatment and resource utilization technologies of municipal waste incineration fly ash: A review. Process Safety and Environmental Protection, 2022. 159: p. 547-565.
16. Xu, L., et al., Status and Development Trend of Harmless and Resourceful Disposal of Municipal Solid Waste Incineration Fly Ash. Adv. Environ. Prot., 2017. 7: p. 414-422.
17. Zhang, Y., et al., Treatment of municipal solid waste incineration fly ash: State-of-the-art technologies and future perspectives. Journal of Hazardous Materials, 2021. 411: p. 125132.
18. De Boom, A. and M. Degrez, Belgian MSWI fly ashes and APC residues: a characterisation study. Waste management, 2012. 32(6): p. 1163-1170.
19. Wongsa, A., et al., Use of municipal solid waste incinerator (MSWI) bottom ash in high calcium fly ash geopolymer matrix. Journal of Cleaner Production, 2017. 148: p. 49-59.
20. Phua, Z., et al., Characteristics of incineration ash for sustainable treatment and reutilization. Environmental Science and Pollution Research, 2019. 26.
21. Chandler, A.J., et al., Municipal solid waste incinerator residues. 1997: Elsevier.
22. Mangialardi, T., Disposal of MSWI fly ash through a combined washing-immobilisation process. Journal of Hazardous Materials, 2003. 98(1-3): p. 225-240.
23. Chen, L., et al., Sustainable stabilization/solidification of municipal solid waste incinerator fly ash by incorporation of green materials. Journal of Cleaner Production, 2019. 222: p. 335-343.
24. Liu, Z., et al., Ash fusion characteristics of bamboo, wood and coal. Energy, 2018. 161: p. 517-522.
25. Tang, P., et al., Immobilization of hazardous municipal solid waste incineration fly ash by novel alternative binders derived from cementitious waste. Journal of hazardous materials, 2020. 393: p. 122386.
26. Cristelo, N., et al., Recycling municipal solid waste incineration slag and fly ash as precursors in low-range alkaline cements. Waste Management, 2020. 104: p. 60-73.
27. Su, X., et al., Evaluation of a flue gas cleaning system of a circulating fluidized bed incineration power plant by the analysis of pollutant emissions. Powder Technology, 2015. 286: p. 9-15.
28. Zhang, M., et al., Stabilization of heavy metals in MSWI fly ash with a novel dithiocarboxylate-functionalized polyaminoamide dendrimer. Waste Management, 2020. 105: p. 289-298.
29. Belevi, H. and H. Moench, Factors determining the element behavior in municipal solid waste incinerators. 1. Field studies. Environmental science & technology, 2000. 34(12): p. 2501-2506.
30. Morf, L.S., P.H. Brunner, and S. Spaun, Effect of operating conditions and input variations on the partitioning of metals in a municipal solid waste incinerator. Waste Management and Research, 2000. 18(1): p. 4-15.
31. Srum, L., F. Frandsen, and J. Hustad, On the fate of heavy metals in municipal solid waste combustion. Part I. devolatilisation of heavy metals on the grate [J]. Fuel, 2003. 82(18): p. 2273-2283.
32. Wu, L., et al., Emission and control characteristics for incineration of Sedum plumbizincicola biomass in a laboratory-scale entrained flow tube furnace. International journal of phytoremediation, 2013. 15(3): p. 219-231.
33. Zhang, Y., et al., Experimental and thermodynamic investigation on transfer of cadmium influenced by sulfur and chlorine during municipal solid waste (MSW) incineration. Journal of Hazardous Materials, 2008. 153(1-2): p. 309-319.
34. Sharifikolouei, E., et al., Vitrification of municipal solid waste incineration fly ash: An approach to find the successful batch compositions. Ceramics International, 2021. 47(6): p. 7738-7744.
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