以三相碳酸化系統探討還原碴封存二氧化碳 之研究

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簡芳瑜(Fang-Yu Chien) 查詢紙本館藏

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論文名稱

以三相碳酸化系統探討還原碴封存二氧化碳之研究
(The Study on Sequestration of Carbon Dioxide by Reductive Slag in a Three-Phase Carbonation System)

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摘要(中)

本研究是以電弧爐還原碴為二氧化碳封存材料，於常溫常壓、總氣體流量1 LPM下進行氣/固/液三相碳酸化反應，藉以探討不同之操作參數，包括固液比、液相鈣離子濃度、二氧化碳濃度、及間歇/連續式通氣，對碳酸化效率及三相碳酸化反應機制的影響。
本研究試驗結果發現，於連續通入二氧化碳氣體情況下，碳酸化效率並非隨固液比增加而增加，其最佳的固液比為20 g/L。當液相鈣離子濃度由500 mg-Ca2+/L提高至1500 mg-Ca2+/L，不僅還原碴中之鈣離子利用率，由78.0%提升至83.3%，且液相含鈣溶液之鈣離子利用率，亦從78.8%升至97.3%，同時在反應系統中，來自兩種不同相態的鈣離子，會與碳酸根產生競爭反應的現象。於間歇式通入二氧化碳氣體情況下，在停止通氣期間，會暫時中斷碳酸化反應，促使還原碴進一步溶出鈣離子，短暫增加漿體中鈣離子濃度。於連續式通氣、12 vol% CO2、0 mg-Ca2+/L的含鈣溶液及固液比30 g/L條件下，操作60分鐘，其三相碳酸化反應之碳酸化效率高達92.2%。
反應動力分析結果顯示，於連續通氣、液相鈣離子濃度為0 mg-Ca2+/L之操作條件下，其反應動力符合表面覆蓋模式，且鈣離子從還原碴中溶出成為速率限制步驟，但隨液相鈣離子濃度增加，其反應動力則會越趨偏離表面覆蓋模式。另一方面，間歇式通氣之三相碳酸化反應，不適合以表面覆蓋模式描述其反應動力行為，表示間歇式通氣系統，可能不會產生碳酸鈣層阻礙還原碴溶出鈣離子。

摘要(英)

The study carried out a gas/solid/liquid three-phase carbonation reaction by using reductive slag as carbon dioxide sequestration material under gas flow rate of 1 LPM at ambient temperature and pressure conditions. The effects of various operation parameters, including solid-liquid ratio, initial calcium concentration in liquid phase, carbon dioxide concentration in gas phase, and intermittent/continuous aeration, on the carbonation efficiency and reaction mechanisms in a three-phase carbonation system were investigated.
The experimental results found that the carbonation efficiency did not increase with the increase of solid-liquid ratio under continuous aeration of carbon dioxide, and the optimum solid-liquid ratio was 20 g/L. When the initial concentration of cal-cium in liquid phase increased from 500 mg-Ca2+/L to 1500 mg-Ca2+/L, not only the calcium utilization efficiency in slag raised from 78.0% to 83.3%, but made calcium utilization efficiency in solution elevated from 78.8% to 97.3%. In addition, the cal-cium came from the different two phases resulted in the competitive phenomenon for carbonate ion in the reaction system. Under intermittent aeration of carbon dioxide, the carbonation reaction was interrupted temporarily during the period of stop-aeration. Consequently, the calcium in slag was further leached out and im-permanent increased the calcium concentration in slurry. Moreover, this study re-vealed that 92.2% carbonation efficiency was achieved under the operation conditions of continuous aeration, 12 vol% of CO2 gas, 0 mg-Ca2+/L of liquid and solid-liquid ratio of 30 g/L at 60 min reaction time in a three phase carbonation system.
The result of reaction kinetics analysis indicated that the reaction of carbona-tion under continuous aeration and 0 mg-Ca2+/L in initial solution conformed to the surface coverage model; also the rate limiting step was the leaching of calcium from slag. However, the fitting degree became lower with the increase of initial calcium in liquid phase. As for three-phase carbonation under intermittent aeration, it was not suitable to describe the reaction kinetics by surface coverage model, because the calcium carbonate layer would not be formed on the slag surface to obstruct the leaching out of calcium ion in slag.

關鍵字(中)

★ 三相碳酸化
★ 還原碴
★ 二氧化碳封存
★ 間歇式通氣
★ 含鈣溶液
★ 表面覆蓋模式

關鍵字(英)

★ three-phase carbonation
★ reductive slag
★ CO2 sequestration
★ intermittent aeration
★ liquid phase with calcium
★ surface coverage model

論文目次

摘要 i
Abstract ii
目錄 iii
圖目錄 vi
表目錄 ix
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 適用封存二氧化碳之材料 3
2-1-1 礦物封存概念 3
2-1-2 選擇材料之依據 4
2-1-3 鋼鐵業爐碴特性 7
2-2 碳酸化反應 10
2-2-1 碳酸化反應之機制與途徑 10
2-2-2 碳酸化反應影響因子 13
2-3 氣固液相碳酸化反應之限制與研究現況 19
2-3-1 反應速率限制步驟 19
2-3-2 近年國內外研究現況 22
2-4 提升碳酸化效率 25
2-4-1 程序強化 25
2-4-2 活化反應物 27
2-5 碳酸化反應動力模式 30
2-5-1 縮核模式(Shrinking Core Model) 30
2-5-2 表面覆蓋模式(Surface Coverage Model) 32
第三章實驗材料與研究方法 34
3-1 研究架構與流程 34
3-2 實驗材料與反應設備 36
3-2-1 實驗材料 36
3-2-2 反應器與主要設備 36
3-3 分析方法與試驗 37
3-3-1 還原碴前處理 37
3-3-2 還原碴物理性質分析 39
3-3-3 還原碴化學性質分析 40
3-3-4 精密儀器分析原理及方法 42
3-4 試驗與實驗方法 45
3-4-1 排序試驗 45
3-4-2 攪動試驗 50
3-4-3 氣固液相碳酸化實驗 50
3-4-4 氣固液相碳酸化效率計算 53
第四章結果與討論 56
4-1 還原碴之特性分析 56
4-1-1 還原碴之物理特性 56
4-1-2 還原碴之化學特性 59
4-2 反應操作建立 61
4-2-1 排序試驗 61
4-2-2 攪動試驗 65
4-3 氣固液相碳酸化反應 69
4-3-1 固液比的影響 70
4-3-2 液相鈣離子濃度的影響 72
4-3-3 二氧化碳濃度的影響 78
4-3-4 間接與連續通氣方式的影響 81
4-3-5 碳酸化反應產物特性 91
4-4 氣固液相碳酸化反應動力模式 97
4-4-1 液相含鈣溶液之碳酸化動力模式 97
4-4-2 間歇式通氣之碳酸化反應動力模式 99
4-5 氣固液相碳酸化反應機制 102
4-5-1 液相含鈣溶液之碳酸化反應機制 102
4-5-2 間歇式通氣碳酸化反應機制 103
第五章結論與建議 105
5-1 結論 105
5-2 建議 107
參考文獻 108
附錄 115

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指導教授

曾迪華(Dyi-Hwa Tseng)

審核日期

2016-4-21

推文