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研究生:廖柏翔
研究生(外文):Bor-Shyang Liao
論文名稱:碳酸鉀和碳酸鈉負載於活性碳吸收煙道氣中二氧化碳之研究:二氧化硫,氮氧化物,氧氣之影響
論文名稱(外文):Absorption of CO2 from Flue Gas by K2CO3 and Na2CO3 Supported on Activated Carbon:Effects of SO2, NOx, and O2.
指導教授:施信民施信民引用關係
指導教授(外文):Shin-Min Shih
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:2009
畢業學年度:97
語文別:中文
論文頁數:177
中文關鍵詞:活性碳碳酸鉀碳酸鈉二氧化碳二氧化硫氮氧化物氧氣碳酸化吸收煙道氣
外文關鍵詞:activated carbonK2CO3Na2CO3CO2SO2NOxO2absorptioncarbonationflue gas
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本研究使用微分固定床反應器,探討於低溫潤濕條件下(60℃,70%RH)SO2、NOx、O2對於碳酸鉀和碳酸鈉負載於活性碳上吸收煙道氣中CO2之影響。在水氣、CO2、SO2、NOx和O2同時存在下,碳酸鉀反應生成碳酸氫鉀、偏重亞硫酸鉀、硫酸鉀、亞硝酸鉀和硝酸鉀;碳酸鈉則生成碳酸氫鈉、亞硫酸鈉、硫酸鈉、亞硝酸鈉和硝酸鈉。碳酸鉀/活性碳吸收劑同時與CO2(12.5%)、NOx(40-600ppm)反應,碳酸化轉化率隨NOx濃度上升而降低,但仍較單獨與CO2(12.5%)反應時為高;同時與CO2和SO2(50-1000ppm)反應,碳酸化轉化率隨SO2濃度上升而降低,但濃度低(≦200ppm)時碳酸化轉化率較單獨與CO2反應時為高。碳酸鈉/活性碳吸收劑同時與CO2和SO2或NOx反應,碳酸化轉化率隨SO2或NOx濃度上升而下降,但在低濃度(≦500ppmSO2或≦100ppmNOx)時,轉化率較單獨與CO2反應時為高。O2(2.5~5.0%)存在與否不影響碳酸鹽/活性碳吸收劑的碳酸化轉化率。一般燃燒廢氣中的SO2和NOx濃度若分別控制在200和300ppm以下,則碳酸鹽/活性碳吸收劑的碳酸化轉化率不低於廢氣中不含SO2和NOx時的轉化率。在相同反應條件下,碳酸鉀/活性碳吸收劑之碳酸化轉化率高於碳酸鈉/活性碳吸收劑。吸收劑可再生利用,其反應性劣化速率緩慢。
A differential fixed-bed reactor was employed to study the effects of SO2, NOx, and O2 on the absorption of CO2 from flue gas by K2CO3 and Na2CO3 supported on activated carbon under low temperature(60℃) and humid conditions(70%RH). With the presence of water vapor, CO2, SO2, NOx, and O2, K2CO3 was converted to KHCO3, K2S2O5, K2SO4, KNO2, and KNO3, and Na2CO3 was converted to NaHCO3, Na2SO3, Na2SO4, NaNO2, and NaNO3. When K2CO3-IAC reacted with CO2(12.5%) and NOx(40-600ppm), the extent of carbonation decreased with increasing NOx concentration, but it was greater than that for the sorbent which reacted with CO2(12.5%) alone.When K2CO3-IAC reacted with CO2 and SO2(50-1000ppm), the extent of carbonation decreased with increasing SO2 concentration, but when the SO2 concentration was low(≦200ppm), it was greater than that for the sorbent which reacted with CO2 alone. When Na2CO3-IAC reacted with CO2 and SO2 or NOx, the extent of carbonation decreased with increasing SO2 or NOx concentration, but at low concentration of SO2(≦500ppm) or NOx(≦100ppm), the extent of carbonation was greater than that for the sorbent which reacted with CO2 alone. The carbonation of sorbents was not affected by the presence of O2(2.5~5.0%). If the concentrations of SO2 and NOx in the flue gas were reduced to values below 200 and 300 ppm, respectively, the extent of carbonation of a sorbent would not be less than that when both SO2 and NOx were absent. Under the same reaction conditions, the extent of carbonation of K2CO3-IAC was greater than that of Na2CO3-IAC. The reactivities of the sorbents decreased only a little after regeneration.
目錄
中文摘要…………………………………………………………………I Abstract……………………………………………………………….II符號說明…….…………..............…………………….....III圖表索引……………………………………………………………..Ⅳ 第一章 緒論 1
第二章 文獻回顧 6
2-1 潮解現象與潮解相對溼度 6
2-2 活性碳、碳酸鉀及碳酸鈉簡介 7
2-3 碳酸鹽、碳酸鹽/活性碳吸收CO2 8
2-4 碳酸鹽吸收SO2 13
2-5 碳酸鹽吸收NOx 18
2-6 碳酸鹽/活性碳吸收NOx/SO2 19
2-7 碳酸鹽活性碳吸收CO2/SO2………………………………………….21 2-8 碳酸鹽、碳酸鹽/活性碳吸收CO2/SO2/NOx/O2………………………23
2-9 碳酸鹽/活性碳吸收劑製備方法 25
第三章 實驗方法 27
3-1 試料來源及吸收劑製備過程 27
3-1-1 試料來源 27
3-1-2 吸收劑製備過程 30
3-1-2-1 K2CO3-IAC吸收劑製備過程 30
3-1-2-2 Na2CO3-IAC吸收劑製備過程 32
3-2 吸收劑物性及化性分析 32
3-2-1 粒徑分析 32
3-2-2 真實密度測量 33
3-2-3 體密度與孔隙度測量 33
3-2-4 BET比表面積及孔隙體積分佈測定 33
3-2-5 熱重分析(TGA) 34
3-2-6 X射線繞射分析(XRD) 34
3-2-7 掃瞄式電子顯微鏡分析(SEM) 34
3-2-8 原子吸收光譜儀分析(AA) 35
3-2-9 離子層析(IC) 38
3-3 反應實驗 38
3-3-1 反應實驗裝置 38
3-3-1-1蒸汽供應系統 44
3-3-1-2 氣體進料系統 45
3-3-2 反應實驗步驟 48
3-3-3 吸收劑轉化率測定 49
3-3-3-1 碳酸鹽負載量 49
3-3-3-2 硫酸化轉化率 51
3-3-3-3 硝酸化轉化率 55
3-3-3-4 碳酸化轉化率 56
第四章 結果與討論 63
4-1 K2CO3-IAC吸收劑結構性質及其反應 63
4-1-1 吸收劑粒徑和密度 63
4-1-2 吸收劑孔隙體積分布與BET比表面積 63
4-1-3 TGA熱重分析 67
4-1-4 X-ray繞射分析(XRD) 78
4-1-5 掃描式電子顯微鏡SEM觀察 85
4-1-5-1 K2CO3-IAC吸收劑與CO2/O2反應 85
4-1-5-2 K2CO3-IAC吸收劑與CO2/SO2/O2反應 88
4-1-5-3 K2CO3-IAC吸收劑與CO2/NOx/O2反應 93
4-1-5-4 K2CO3-IAC吸收劑與CO2/SO2/NOx/O2反應 93
4-1-6 K2CO3-IAC吸收劑與廢氣成份之反應 99
4-1-6-1 K2CO3-IAC吸收劑與CO2反應 99
4-1-6-2 K2CO3-IAC吸收劑與CO2/O2反應 102
4-1-6-3 K2CO3-IAC吸收劑與CO2/SO2反應 108
4-1-6-4 K2CO3-IAC吸收劑與CO2/SO2/O2反應 110
4-1-6-5 K2CO3-IAC吸收劑與CO2/NOx反應 111
4-1-6-6 K2CO3-IAC吸收劑與CO2/NOx/O2反應 112
4-1-6-7 K2CO3-IAC吸收劑與CO2/SO2/NOx反應 112
4-1-6-8 K2CO3-IAC吸收劑與CO2/SO2/NOx/O2反應 113
4-2 Na2CO3-IAC吸收劑結構性質及其反應 114
4-2-1 吸收劑粒徑和密度 114
4-2-2 吸收劑孔隙體積分布與BET比表面積 114
4-2-3 TGA熱重分析 117
4-2-4 X-ray繞射分析(XRD) 128
4-2-5 掃描式電子顯微鏡SEM觀察 136
4-2-5-1 Na2CO3-IAC吸收劑與CO2反應 136
4-2-5-2 Na2CO3-IAC吸收劑與CO2/SO2/O2反應 136
4-2-5-3 Na2CO3-IAC吸收劑與CO2/NOx/O2反應 140
4-2-5-4 Na2CO3-IAC吸收劑與CO2/SO2/NOx/O2反應 145
4-2-6 Na2CO3-IAC吸收劑與廢氣成份之反應 145
4-2-6-1 Na2CO3-IAC吸收劑與CO2反應 145
4-2-6-2 Na2CO3-IAC吸收劑與CO2/O2反應 150
4-2-6-3 Na2CO3-IAC吸收劑與CO2/SO2反應 156
4-2-6-4 Na2CO3-IAC吸收劑與CO2/SO2/O2反應 157
4-2-6-5 Na2CO3-IAC吸收劑與CO2/NOx反應 157
4-2-6-6 Na2CO3-IAC吸收劑與CO2/NOx/O2反應 157
4-2-6-7 Na2CO3-IAC吸收劑與CO2/SO2/NOx反應 158
4-2-6-8 Na2CO3-IAC吸收劑與CO2/SO2/NOx/O2反應 158
4-3 吸收劑反應性之比較與討論 159
4-3-1 K2CO3-IAC吸收劑之低溫潤濕反應比較 159
4-3-2 Na2CO3-IAC吸收劑之低溫潤濕反應比較 161
4-4 吸收劑之再生性 161
4-4-1 K2CO3-IAC吸收劑之再生性……………………….……..161
4-4-2 Na2CO3-IAC吸收劑之再生性……….………………...….164
第五章 結論 167
參考文獻 169
附錄 174
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