鋼鐵業副產物衍生磷酸陶瓷固化劑之研究

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林漢宗(Han-Zong Lin) 查詢紙本館藏

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論文名稱

鋼鐵業副產物衍生磷酸陶瓷固化劑之研究
(Study on Developing CBPC Stabilizer using Steel Making Wastes)

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摘要(中)

本研究針對電弧爐集塵灰、高爐礦泥、鑄鐵集塵灰與熱軋礦泥等鋼鐵鑄造業副產物具有微細顆粒與含有大量氧化鐵之特性，以及晶圓廠廢磷酸的穩定化特性，經由化學計量式與試拌程序混合產製磷酸陶瓷固化劑，並探討磷酸濃度與硼酸劑量對固化體之性質影響實驗，獲得固液比等磷酸陶瓷固化劑配方；同時，以各類固化劑配方固化不同劑量的飛灰，探討飛灰固化量對磷酸陶瓷固化體的新拌與硬固性質，溶出特性，以及微結構的影響，藉此獲得各類磷酸陶瓷固化體的最佳飛灰固化量。最後，以水泥固化為比較基準對各類固化劑進行經濟效益評估。
實驗結果顯示電弧爐集塵灰、高爐礦泥、鑄鐵集塵灰與熱軋礦泥的化學組成會與磷酸產生明顯反應的氧化金屬總含量，以電弧爐集塵灰與熱軋礦泥為較高(達54%)，高爐礦泥次之(38%)，鑄鐵集塵灰最低(35%)。前述此四類磷酸陶瓷固化劑的配方：每克鋼鐵業副產物需要磷酸量分別為0.84克、0.68克、0.68克與0.98克，固液比分別為0.52、0.60、0.80與0.30；最佳的硼酸緩凝劑使用量為2wt.%。磷酸濃度過高可能因激烈發泡反應而對固化體的新拌與硬固性質產生不利影響，建議適當磷酸濃度應低於75%以下，而不宜過高。此四種磷酸陶瓷飛灰固化體之TCLP結果均符合法規值，對於Pb與Cu的穩定效果最佳，但部分固化體的抗壓強度低於法規值；電弧
爐集塵灰、高爐礦泥、鑄鐵集塵灰等磷酸陶瓷固化體之最大飛灰固化量分別為20%、25%、30%，而熱軋礦泥磷酸陶瓷固化體則不適合應用於固化飛灰。電弧爐集塵灰與鑄鐵集塵灰兩種磷酸陶瓷固化劑比傳統水泥固化劑
深具經濟性，因此具有資源化與市場競爭潛力。

摘要(英)

Chemically bonded phosphate ceramics (CBPCs) are produced by acid-base reactions between an inorganic oxide and either phosphoric acid solution or an acid-phosphate solution. By taking the advantage of forming chemical phosphate bond and the ability to capsulate wastes, the CBPCs can be used to solidify and/or stabilize toxic wastes. Typical reactants of this acid-base process (i.e., MgO, Fe2O3, and phosphoric acid) can be provided with by industrial wastes: iron-oxide-containing wastes can be obtained from steel making plants, and waste phosphoric acid from IC foundry plants. Some of the iron oxide may also be obtained from the MSWI fly ash. These industrial wastes provide an excellent opportunity to evaluate the feasibility of developing phosphate ceramics from wastes (referred to as WDPCs), and to assess their further applicability to solidify and/or stabilize MSWI fly ash. Accordingly, this study investigated the feasibility of developing phosphate ceramics from wastes such as electric arc furnace dust (EAF dust), blast furnace wet dust (BF dust), cast iron dust (CI dust), and hot-roll wet dust (HR dust); as well as waste phosphoric acid. In this study, the waste-derived
phosphate ceramics (WDPCs) were further evaluated by their capacity to solidify and/or stabilize MSWI fly ash.
The results indicate that the reactive inorganic oxides, mainly iron (III) oxide, in EAF dust, BF wet dust, CI dust, and HR wet dust were found to be 54, 38, 35, and 54% (w/w), respectively. Each gram of the dusts, stoichiometrically, required 0.84, 0.68, 0,68, and 0.98 gram of phosphoric acid (pure) respectively to produce proper WDPCs, or 1.53, 1.24, 1.24, and 1.77 gram for phosphoric acid of averaged 55% concentration. The WDPCs were fabricated by adding water to the previous formula at a solid-to-liquid ratio as determined by a workable viscosity of the WDPC pastes. The
determination resulted in an appropriate solid- to-liquid ratio of 0.52, 0.60, 0.80, and 0.30, respectively for the tested EAF dust, BF dust, CI dust, and HR dust respectively. Phosphoric acid concentration less than 75% was recommended to avoid vigorous acid-base reaction and the excessive forming, which adversely affected the quality of the WDPC pastes. For all WDPC samples, the leaching concentrations of the target metals resulting from the TCLP test were found to be in compliance with the US EPA’’s regulatory thresholds. The effect of solidification/stabilization for Pb and Cu was especially significant. However, some WDPCs failed to develop sufficient regulatory compressive strength for solidified monolith. One the other hand, of the four WDPCs tested, the
maximum ratio for MSWI fly ash to be solidified was found to be 20, 25, and 30% (w/w) for phosphate ceramics derived from the corresponding EAF dust, BF dust, and CI dust; whereas that derived from HR wet dust failed in
solidifying/stabiling MSWI fly ash.
Solidification/stabilization of MSWI fly ash with WDPCs is economically competitive with other disposal methods such as traditional cement
solidification process and can have the added attractiveness of being beneficial to the waste disposal.

關鍵字(中)

★ 焚化飛灰
★ 鋼鐵業副產物
★ 磷酸陶瓷
★ 固化劑

關鍵字(英)

★ steel industry waste
★ Chemically Bonded Phosphate
★ MSWI fly ash

論文目次

目錄
第一章前言·································································1
1-1 研究緣起與目的···························································1
1-2 研究內容·································································2
第二章文獻回顧······························································3
2-1 都市垃圾焚化飛灰的來源與性質·············································3
2-1-1 飛灰產源及產量·······························3
2-1-2 飛灰物化特性···························································5
2-1-3 飛灰之化學元素分布特性·················································8
2-2 傳統固化與穩定化之文獻回顧··············································12
2-2-1 固化/穩定化原理······························12
2-2-2 磷酸穩定化相關文獻回顧················································15
2-3 磷酸陶瓷的發展背景與應用················································18
2-3-1 磷酸陶瓷的發展背景····················································18
2-3-2 磷酸陶瓷的特色························································18
2-3-3 磷酸陶瓷的應用範圍····················································20
2-4 磷酸陶瓷固化的原理與影響因子············································26
2-4-1 二價氧化金屬原料·····························26
2-4-2 三價氧化金屬原料·····························28
2-4-3 溶解度··································30
2-4-4 顆粒比表面積對於反應之影響············································34
2-4-5 影響因子······························································35
第三章實驗材料與方法·······················································37
3-1 實驗流程································································37
3-2 實驗配置································································40
3-2-1 磷酸陶瓷固化劑配方實驗················································40
3-2-2 硼酸用量實驗··························································40
3-2-3 磷酸濃度實驗··························································41
3-2-4 飛灰固化量配比試驗····················································41
3-3 實驗材料與方法··························································42
3-3-1 實驗材料·································42
3-3-2 實驗與分析設備························································53
3-4 實驗操作································································55
3-4-1 前處理··································55
3-4-2 試體的製備與養護······················································55
3-5 實驗分析································································58
第四章結果與討論································67
4-1 飛灰與各類廢棄物衍生磷酸陶瓷原料的基本性質······························67
4-1-1 物理性質······························································67
4-1-2 化學特性······························································76
4-1-3 重金屬總量與溶出特性··················································79
4-1-4 物種型態與微觀結構····················································81
4-1-5 總結··································································88
4-2 前置試驗································································89
4-2-1 磷酸陶瓷固化劑之配方··················································89
4-2-2 磷酸陶瓷固化劑之固液比················································91
4-2-3 硼酸劑量對新拌漿體性質之影響··········································96
4-3 磷酸濃度試驗···························································100
4-3-1 磷酸濃度對新拌漿體之性質影響·········································100
4-3-2 磷酸濃度對固化體之物化性質影響·······································104
4-3-3 磷酸濃度對固化體之微結構影響·········································110
4-3-4 總結·································································118
4-4 磷酸陶瓷固化飛灰實驗···················································120
4-4-1 飛灰固化量對新拌漿體之性質影響·······································120
4-4-2 飛灰固化量對磷酸陶瓷固化體之物理性質影響·····························134
4-4-3 飛灰固化量對固化體之重金屬溶出特性與耐水性影響·······················150
4-4-4 飛灰固化量對磷酸陶瓷固化體之微觀結構影響·····························195
4-4-5 總結·································································215
4-5 磷酸陶瓷固化劑經濟性分析···············································220
第五章結論與建議···························································225
5-1 結論····································225
5-2 建議···································································229
參考文獻···································································230

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指導教授

王鯤生(Kuen-Sheng Wang)

審核日期

2005-7-22

推文