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研究生:張耿豪
研究生(外文):Chang Keng-Hao
論文名稱:添加劑對石灰石與二氧化硫低溫反應之影響
論文名稱(外文):Effects of Additives on the Reaction of Limestone with SO2 at Low Temperatures
指導教授:施信民施信民引用關係
指導教授(外文):Shinh Shin-Min
學位類別:碩士
校院名稱:國立臺灣大學
系所名稱:化學工程學研究所
學門:工程學門
學類:化學工程學類
論文種類:學術論文
論文出版年:2002
畢業學年度:90
語文別:中文
論文頁數:110
中文關鍵詞:煙道氣除硫二氧化硫石灰石添加劑
外文關鍵詞:Flue gas desulfurizationLimestoneSulfur dioxideAdditives
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中文摘要
本研究在模擬噴霧乾燥法煙道氣除硫系統之袋式集塵器之條件下,以微分固定床反應器探討添加劑對石灰石與二氧化硫低溫反應之影響。石灰石來自花蓮和平地區,經由溼式研磨而得不同比表面積的試樣。所用添加劑為NaOH、Na2CO3、K2CO3、LiCl、NaCl、KCl、CaCl2、NaNO2、NaNO3、Na2SO3、Na2SO4,皆為潮解鹽。添加添加劑之石灰石是將兩者加水混合,再經乾燥而得乾燥試樣,其中添加劑含量為1至10mol%。
由於潮解鹽使得石灰石吸收劑在相同溼度下能吸收比未添加時更多的水氣,因此能增進初期反應速率及一小時轉化率,反應速率及轉化率隨相對溼度和添加量增加而增加。在60℃、70%RH和1000ppmSO2下反應一小時,添加劑(5mol%)對石灰石的轉化率提升程度的大小順序為CaCl2>KCl>NaCl>NaNO3>LiCl>Na2CO3>NaOH>K2CO3>Na2SO4>NaNO2>Na2SO3,這些試樣轉化率皆比未添加的石灰石或氫氧化鈣高。
在高相對溼度下,添加氯化鈣之石灰石與二氧化硫反應的速率隨二氧化硫濃度增加而增加,但反應溫度及石灰石之初始比表面積的影響並不顯著。在有氧氣或氮氧化物時,添加氯化鈣之石灰石硫酸化的產物為CaSO3.1/2H2O 和CaSO4˙2H2O,若無氧氣或氮氧化物時,產物為CaSO3.1/2H2O。
石灰石添加適當之潮解鹽可以取代氫氧化鈣作為乾式或半乾式除硫程序之吸收劑。
Abstract
A differential fixed-bed reactor was employed to study the effects of additives on the reaction between limestone and SO2 under the conditions similar to those in the bag filters of the spray-drying flue gas desulfurization system. Limestone was from Her-Ping, Hualien. Samples of different specific surface areas were prepared by wet grinding. Additives used were deliquescent salts, NaOH, Na2CO3, K2CO3, LiCl, NaCl, KCl, CaCl2, NaNO2, NaNO3, Na2SO3, and Na2SO4. A salt (1 to 10mol%) as added to limestone by slurrying and drying processes.
All the salts enhanced the reaction of limestone with SO2 because the salts adsorbed more water. The initial reaction rate and one hour conversion of limestone with a salt added increased as relative humidity or the amount of the salt increased. At 60℃, 70%RH, 1000ppmSO2, and 1h, the ranking of the effect of salt on the conversion of limestone with 5mol% salt added was CaCl2>KCl>NaCl>NaNO3>LiCl>Na2CO3>NaOH>K2CO3>Na2SO4>NaNO2>Na2SO3;at the reaction conditions, the conversion of limestone with a salt added was higher than that of CaCO3 or Ca(OH)2 without the salt added.
For limestone with CaCl2 added, the reaction rate increased with SO2 concentration at high relative humidity, but the effects of temperature and the initial BET surface area of limestone were absent. The reaction products of limestone with CaCl2 added were found to be CaSO3.1/2H2O and CaSO4.2H2O under the presence of NOx and O2 in the gas mixture, and CaSO3.1/2H2O without the presence of NOx and O2.
Limestone added with proper deliquescent salts can replace Ca(OH)2 as a sorbent for the dry or semidry flue gas desulfurization processes.
目錄 Page
中文摘要…………………………………………………………. I
Abstract…………………………………………………………... III
符號說明…………………………………………………………. V
圖表索引…………………………………………………………. VII
第一章 緒論……………………………………………………... 1
第二章 文獻回顧……………………………………………….. 5
2-1 石灰石性質………………………………………………… 5
2-2 石灰石與二氧化硫在低溫潤濕條件下的反應………………… 6
2-3 氣體成分對氫氧化鈣和石灰石反應性影響…………………… 9
2-4 添加劑對氫氧化鈣與石灰石吸硫反應性的影響………………… 13
2-5 潮解鹽和潮解現象……………………………………………. 14
第三章 實驗與分析方法……………………………………... 19
3-1 試料來源及藥品………………………………………………. 19
3-2 吸收劑製備程序………………………………………………. 21
3-3 反應實驗裝置………………………………………………… 21
3-4 反應實驗步驟………………………………………………… 28
3-5 試樣物性與化性分析………………………………………….. 30
3-6 石灰石轉化率之測定………………………………………… 32
第四章 結果與討論…………………………………………….. 39
4-1 微分床操作條件的驗證……………………………………… 39
4-2 添加劑促進石灰石反應性之效果比較………………………... 41
4-3 吸收劑之水吸附…………………………………………….. 44
4-4 添加劑莫耳分率對吸收劑反應性的影響………………………… 46
4-5 反應溫度的影響………………………………………………. 48
4-6 相對溼度對吸收劑反應性的影響………………………………. 50
4-7 二氧化硫濃度對吸收劑反應性的影響………………………….. 55
4-8 比表面積對吸收劑反應性的影響………………………………. 57
4-9 煙道氣體的影響……………………………………………… 64
4-10 含添加劑之石灰石與Ca(OH)2對二氧化硫之反應性比較……….. 68
4-11 物性分析……………………………………………………... 74
第五章 結論…………………………………………………….. 104
參考文獻…………………………………………………………. 107
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