利用水處理污泥合成活性碳-沸石複合材料同時去除染料與重金屬之研究

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陳雅馨(Ya-sing Chen) 查詢紙本館藏

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環境工程研究所

論文名稱

利用水處理污泥合成活性碳-沸石複合材料同時去除染料與重金屬之研究
(Study on synthesis of activated carbon-zeolite composites from water treatment sludge and their applications)

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摘要(中)

本研究主要探討利用下水污泥與淨水污泥灰作為碳及矽、鋁源，以鹼熔與水熱兩階段程序合成活性碳-沸石複合吸附材料，並藉由有機及無機污染物吸附試驗來評估其作為環境淨化資材之可行性。複合吸附材料製備過程是以混合不同比例之下水污泥與淨水污泥灰，來配置污泥原料中之Si/Al莫耳比與碳含量，進而探討其對複合吸附材料中沸石結晶物種之影響。實驗結果證實影響沸石結晶物種之主要因子為原料之Si/Al莫耳比。下水污泥與淨水污泥灰之混合比例1:9之原料理論Si/Al為1.57，所製備出複合材料ACZ1090為低活性碳含量之純相Na-A型沸石；而混合比例為3:7之ACZ3070與5:5之ACZ5050原料之理論Si/Al分別為1.72與1.93，所製備出之兩複合材料活性碳含量則分別為2.75 %及4.14 %，而主要沸石結晶物種皆為Na-X型沸石。等溫吸附試驗結果，發現三組以不同混合比例之水處理污泥所製備出的活性碳-沸石複合吸附材料ACZ1090、ACZ3070及ACZ5050個別吸附MB、Cu(II)、Cd(II)皆符合Langmuir模式，而複合吸附材料ACZ1090對MB、Cu(II)及Cd(II)之最大吸附量依序為0.10、0.68、0.49 mmole/g；ACZ3070為0.11、0.64、0.50 mmole/g；ACZ5050則為0.14、0.56、0.45 mmole/g。而在多成份污染物吸附試驗發現三組以水處理污泥為原料所製備出的複合吸附材料對污染物之吸附選擇性順序為Cu(II)＞Cd(II)＞MB。最後，比較市售沸石與自製複合吸附材料之污染物去除能力，確定以水處理污泥所製備出之活性碳-沸石複合吸附材料具有一定之污染物去除效力，確實可作為環境淨化資材。

摘要(英)

This study investigated the feasibility of synthesizing activated carbon-zeolite composites (AC-Z composites), using primarily sewage and water purification sludge as starting silicon, aluminum and carbon sources; and the AC-Z composites as synthesized in this study were evaluated for their adsorption behavior of Cd, Cu and methylene blue (MB), in hope that such composites could be applied to remove organic and inorganic pollutants simultaneously.
Firstly, the starting sludges as received were pretreated by drying and/or incineration to provide the dry sewage sludge (DSS) and the water purification sludge ash (WPSA), respectively, for the subsequent study. Secondly, it is supposed that the silicon and aluminum sources are provide by both DSS and WPSA, and the carbon source solely by DSS, and that the molar ratio of Si/Al and carbon content can affect the synthesis of zeolite and production of activated carbon; therefore, starting materials with various Si/Al ratio and carbon content were prepared by a mix design of DSS and WPSA (i.e., DSS:WPSA=1:9, 3:7 and 5:5). Thirdly, the synthesis of AC-Z composites were conducted by an alkali fusion, followed by a hydrothermal process.
The results indicate that the resultant ACZ1090 composite ( i.e., DSS:WPSA=1:9 for the starting mixture) was confirmed to contain trace amount of activated carbon and single-phased Na-A zeolite as main phase; in contrast, ACZ3070 composite, 2.75% activated carbon and Na-X zeolite as main phase; and ACZ5050 composite, 4.14% activated carbon and Na-X zeolite also as main phase. The results suggest that the activated carbon content in the resultant composites increased with increasing mix portion of DSS; and the theoretical Si/Al ratio of the starting mixture increased with the increasing portion of DSS (i.e., from 1.57 to 1.93), it seemed that with the increasing Si/Al ratio, the main crystal phase of in the resultant composites shifted from Na-A type to Na-X type.
The resultant AC-Z composites were evaluated for their adsorption of MB, Cu(II) and Cd(II). The adsorption of MB, Cu(II) and Cd(II), respectively, in a single component system, was found well fitted with the Langmuir model. The maximum adsorption of MB, Cu(II) and Cd(II), in a single component system was found to be 0.10, 0.68 and 0.49 mmole/g, respectively for ACZ1090 composite; and in comparison, 0.11, 0.64 and 0.50 mmole/g, respectively, for ACZ3070 composite; and 0.14, 0.56 and 0.45 mmole/g, respectively, for ACZ5050 composite. All the adsorption performance was comparable to that of the commercial grade 4A zeolite and 13X zeolite. However, the adsorption of MB, Cu(II) and Cd(II), in a multi-component system showed decreased adsorption quantity for the tested adsorbates, possibly due to the competition among the adsorbates. It was found that the selectivity for the tested adsorbates in decreasing order was Cu(II)>Cd(II)>MB.
This work demonstrated that it is feasible and beneficial to synthesize activated carbon-zeolite composites (AC-Z composites) with primarily sewage and water purification sludge as starting silicon, aluminum and carbon sources. The results may contribute to the recycling of water treatment sludges and the production of green activated carbon-zeolite composites.

關鍵字(中)

★ 下水污泥
★ 淨水污泥
★ 活性碳
★ 沸石
★ 吸附

關鍵字(英)

★ Water Purification Sludge
★ Primarily Sewage Sludge
★ Activated carbon
★ Zeolite
★ Adsorption

論文目次

誌謝 i
中文摘要 ii
英文摘要 iii
目錄 v
圖目錄 viii
表目錄 x
第一章前言 1
1-1 研究緣起 1
1-2 研究目的 2
第二章文獻回顧 3
2-1 水處理污泥 3
2-1-1 水處理污泥來源及產量 3
2-1-2 水處理污泥之組成特性 6
2-1-3 水處理污泥之處理現況 7
2-2 染料與重金屬 8
2-2-1 染料、銅與鎘之來源 8
2-2-2 去除染料與重金屬之方法 8
2-3 沸石簡介 10
2-3-1 沸石發展史 10
2-3-2 沸石結構特性與分類 10
2-3-3 沸石之製備方法 12
2-4 合成沸石或活性-沸石複合吸附材料之相關研究 13
2-4-1 沸石或活性碳-沸石複合吸附材料之製備方法 13
2-4-2 影響沸石結晶物種之操作參數 19
2-5 吸附理論 21
2-5-1 物理吸附與化學吸附 21
2-5-2 等溫吸附分類 21
2-5-3 等溫吸附方程式 23
第三章研究材料與方法 25
3-1 研究架構 25
3-2 實驗材料與設備 27
3-2-1 實驗材料 27
3-2-2 實驗用藥品 29
3-2-3 實驗設備 30
3-3 實驗設計 32
3-3-1 原物料前處理 32
3-3-2 水處理污泥合成活性碳-沸石複合吸附材料試驗 32
3-3-3 吸附試驗 34
3-4 實驗條件配製 35
3-4-1 製備活性碳-沸石複合吸附材料之實驗配置 35
3-4-2 吸附試驗之實驗配置 36
3-5 實驗分析儀器與方法 37
3-5-1 分析儀器 37
3-5-2 分析方法 42
第四章結果與討論 45
4-1 下水污泥以及淨水污泥灰之基本性質分析4 5
4-1-1 水處理污泥之物化性質分析 45
4-1-2 水處理污泥之重金屬總量毒性溶出試驗 47
4-1-3 水處理污泥之結晶相物種分析 48
4-1-4 水處理污泥之微結構特性分析 50
4-2 鹼熔與水熱兩階段程序合成活性碳-沸石複合材料 51
4-2-1 不同混合比例之水處理污泥對鹼熔產物之影響 51
4-2-2 不同混合比例之水處理污泥對水熱最終產物之影響 54
4-2-3 小結 57
4-3 活性碳-沸石複合吸附材料之基本性質分析 59
4-3-1 活性碳-沸石複合吸附材料化學組成分析 59
4-3-2 活性碳-沸石複合吸附材料氮氣吸/脫附分析 61
4-3-3 活性碳-沸石複合吸附材料傅立葉轉換紅外線光譜分析 66
4-3-4 活性碳-沸石複合吸附材料微結構特性分析 68
4-4 吸附試驗 71
4-4-1 單成份吸附試驗 71
4-4-2 多成份吸附試驗 79
第五章結論與建議 81
5-1 結論 81
5-2 建議 84
參考文獻 85

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指導教授

王鯤生(Kuen-sheng Wang)

審核日期

2011-10-27

推文