利用改質氧化鈣吸附二氧化碳之效率探討

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曾怡玲(Chen-yi Lin) 查詢紙本館藏

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論文名稱

利用改質氧化鈣吸附二氧化碳之效率探討
(Investigation on CO2 capture efficiencies achieved with modified calcium oxides materials)

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摘要(中)

隨著地球暖化逐漸加劇，降低CO2排放為現今世界各國努力的目標，而發展CO2捕獲關鍵技術為減排技術之重要研究方向。中高溫捕獲CO2可降低能損，並具有吸附質含量高(約10-15% CO2)之優點，此技術又以含氧化鈣材料最具有優勢。因此，利用高性能吸附材料進行CO2捕獲，未來也必然成為重要趨勢之一。文獻指出高溫劣化為氧化鈣捕獲CO2之缺點，將嚴重降低捕碳劑之長期穩定性。
本研究針對二氧化碳捕捉技術開發，探討含氧化鈣中高溫吸附材料製備及其CO2吸脫附效率。利用共沉法將三種鈣離子前驅物與鋁離子前驅物共沉後，再經由高溫煅燒處理，以生成層狀Ca-Al-CO3吸附劑。同時針對自製層狀Ca-Al-CO3吸附劑進行BET、XRD、SEM 等特性分析及利用TGA 測試CO2吸附效率，以進行二氧化碳吸附效能之評估。結果顯示三種吸附劑係為中孔洞吸附劑之吸附行為。由實驗結果得知，三種吸附劑最適吸附溫度皆落在750°C，起始吸附量以(Ca-Al-CO3/CaO) (55.8%)最高，其次Ca(OAc)2-LDH (52.1%)，最差者為Ca(NO3)2-LDH (46.9%)。(Ca-Al-CO3/CaO)不但具有最佳的捕碳性能，經過40 次的吸脫附測試後，仍維持96%穩定性之優越性能。未來若能將此技術用於含氧化鈣之礦物改質，將成為極具有潛力之碳捕獲技術。
關鍵字：二氧化碳捕獲；吸附劑；氧化鈣；Ca-Al-CO3；熱重分析

摘要(英)

Combustion of fossil fuel causes increasing atmospheric CO2 concentration and induces man-made greenhouse effect, hence, developing effective technique for CO2 capture to mitigate its emission has become an important issue. The medium-high temperature CO2 capture technique has the major advantage of decreasing the energy penalty and is of a high capture efficiency at a high CO2 concentration (ca. 15-50%CO2). Material containing CaO is a promising candidate for adsorbing CO2 under elevated temperature, which should be a promising trend in the future. Previous study indicates that the sintering of CaO at high temperature is the major reason for the decay of CO2 capture, resulting in the poor stability of sorbent. This research aims to develop an effective CO2 capturing technology via the preparation and testing of CaO-based layer double hydroxides (LDHs) sorbents. This study focuses on the development of a Ca-Al-CO3 sorbent derived from three kinds of precursors: (I) (Ca-Al-CO3/CaO) (II) Ca(OAc)2-LDH and (III) Ca(NO3)2-LDH. Ca+2 ions are incorporated into layered structure by co-precipitation of Al (NO3)3•9H2O and Na2CO3 under alkaline conditions. The characteristics of synthesized sorbents such as surface area, morphology/particle size and crystalline are determined by BET (Quantachrome), SEM (Hitachi) and PXRD (Bruker), respectively. Sorption properties of CO2 on CaO are monitored by recording weight change of sorbent with a Thermo-gravimetric analyzer (TGA, Netzsch) operated at alternately cycling experiments of adsorption and desorption for CO2 capture. The results showed that the microscopic characters of sorbents were mainly mesoporous. CO2 sorption capacities (g CO2/g sorbent) at 750 °C were in the range of 0.524-0.672 and they were significantly related to sorbents, wherein (Ca-Al-CO3/CaO) (55.8%) >Ca(OAc)2-LDH (52.1%) > Ca(NO3)2-LDH (46.9%). The best Ca-Al-CO3 sorbent was from (Ca-Al-CO3/CaO) that provided at least 96% CO2 sorption recovery after 40 adsorption/desorption cycles. These materials are worthy to be further studied for the modification of alkaline minerals as a potential CO2 sorbent.
Keywords: CO2 capture; Adsorbents; CaO; Ca-Al-CO3 ; Thermal gravimetric analysis(TGA).

關鍵字(中)

★ 二氧化碳捕獲
★ 吸附劑
★ 氧化鈣
★ 熱重分析

關鍵字(英)

★ CO2 capture
★ Ca-Al-CO3
★ Adsorbents
★ Thermal gravimetric analysis

論文目次

摘要 i
Abstract iii
致謝 v
目錄 vi
圖目錄 xi
表目錄 xiii
第一章前言 1
1.1研究起緣 1
1.2研究目的 3
第二章文獻回顧 5
2.1溫室效應簡介 5
2.1.1溫室效應 5
2.1.2溫室效應氣體 6
2.2二氧化碳捕獲路徑 7
2.2.1 燃燒後捕獲 8
2.2.2 燃燒前捕獲 8
2.2.3 富氧燃燒 9
2.3二氧化碳捕獲技術 10
2.3.1 化學方式 10
2.3.2 物理方式 11
2.4 二氧化碳吸附材料簡介 13
2.4.1 固體吸附劑特性 16
2.4.2 層狀水滑石 (Layered double hydroxide, LDH) 20
2.5 吸附材料之選擇 21
2.5.1 中高溫吸附材料 22
2.5.2 吸附材料 (吸附劑) 所需特性 23
2.6 氧化鈣改質之探討 24
第三章實驗方法 29
3.1研究流程 29
3.2實驗設備及藥品 30
3.3材料製備 31
3.4 實驗步驟與方法 33
3.4.1 氧化鈣改質捕碳劑合成-氧化鈣(A吸附劑) 33
3.4.2 含氧化鈣層狀捕碳劑合成-醋酸鈣(B吸附劑) 34
3.4.3 含氧化鈣層狀捕碳劑合成-硝酸鈣(C吸附劑) 35
3.5 吸附劑之鑑定分析 36
3.5.1 TGA 吸附/脫附測試 36
3.5.2 比表面積、孔隙體積及孔徑大小分佈(BET) 37
3.5.3 X 射線繞射(XRD)分析 37
3.5.4 掃描式電子顯微鏡(SEM)形貌觀察分析分析 38
第四章實驗結果與討論 40
4.1 含氧化鈣層狀捕碳劑合成與分析-氧化鈣(A吸附劑) 40
4.1.1 TGA 吸附/脫附測試 40
4.1.2 吸附劑比表面積特性分析(BET) 44
4.1.3 X 射線繞射結構特性(XRD) 46
4.1.4 掃描式電子顯微鏡(SEM) 48
4.2 含氧化鈣層狀捕碳劑合成與分析-醋酸鈣(B吸附劑) 50
4.2.1 TGA 吸附/脫附測試 50
4.2.2 吸附劑比表面積特性分析(BET) 53
4.2.3 X射線繞射結構特性(XRD) 54
4.2.4 掃描式電子顯微鏡(SEM) 56
4.3 含氧化鈣層狀捕碳劑合成-硝酸鈣(C吸附劑) 59
4.3.1 TGA 吸附/脫附測試 59
4.3.2 起始吸附量及穩定性分析 60
4.3.3 吸附劑比表面積特性分析(BET) 62
4.3.4 X 射線繞射結構特性(XRD) 68
4.3.5 掃描式電子顯微鏡(SEM) 70
4.4 三種(A、B、C)吸附劑比較與綜合討論 72
4.4.1 三種(A、B、C)吸附劑比較 72
4.4.2 三種(A、B、C)吸附劑綜合討論 73
4.4.3 三種(A、B、C)吸附劑成本分析及起始吸附之比較 75
4.4.4 三種(A、B、C)吸附劑成本分析及穩定性比較 77
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

張木彬

審核日期

2013-7-25

推文