本論文主要是研究以觸媒還原法處理含二氧化硫及一氧化氮之氣體。首先研製篩選高性能之觸媒，接著我們進行了物性的鑑定和動力學之研究，以及TPR（程溫還原）和TPD（程溫脫附）等實驗。根據實驗及鑑定的結果，我們探究活性、選擇性及穩定性高低之原由，並推測可能之反應機構。除此之外，也探討觸媒預處理及進料中水蒸氣及氧氣對轉化率、生成分率與觸媒穩定性之影響。

　　針對以氫氣為還原劑之二氧化硫還原反應，首先測試以γ-Al2O3為擔體之單金屬氧化物（Fe2O3、NiO、MnO2、MoO3、Cr2O3、Co3O4、CuO ）觸媒中，發現NiO/γ-Al2O3觸媒對二氧化硫還原反應具最佳活性，Co3O4/γ-Al2O3觸媒次之。再將硝酸鎳溶液含浸於五種不同擔體上（γ-Al2O3、SiO2、TiO2、CeO2、V2O5 ），製成五種NiO擔體觸媒，結果以NiO/γ-Al2O3觸媒活性最佳。改變鎳含量，發現鎳含量為16 wt% 之NiO/γ-Al2O3擔體觸媒具有最佳活性。在不同進料莫爾比 ( H2/SO2 =1~4 ) 之下反應，發現H2/SO2 進料莫爾比為2是最佳進料條件。若以H2S+H2、H2、He等氣體對NiO/γ-Al2O3觸媒作前處理，發現以通入H2S+H2氣體作為前處理氣體可獲得最佳活化效果。進料之反應物中含水，對觸媒活性有抑制作用但為可逆。XRD測定結果發現，活性金屬硫化鎳在反應過程中，由有硫空缺之NiS及Ni3S2轉變為NiS2。

　　接著以溶膠凝膠法製備奈米級CeO2，再以臨濕含浸法將金屬鹽類化合物分別含浸於奈米級CeO2 擔體上，製備各種不同奈米級金屬氧化物擔體觸媒。並利用TEM、SEM及XRD等儀器進行擔體及觸媒之組成與表面性質測定。實驗結果發現以溶膠凝膠法製備之擔體觸媒的顆粒介於20-50 nm。接著將這些擔體觸媒用來作為以一氧化碳 ( CO ) 為還原劑將二氧化硫 ( SO2 ) 還原為元素硫的研究。實驗結果顯示Cr2O3 /nano-CeO2 擔體觸媒最具活性。我們繼續以Cr2O3 /nano-CeO2 擔體觸媒進行SO2還原反應之研究，結果顯示CO和SO2 最適當的進料比為2.5，且SO2 和CO若濃度低，則SO2 的轉化率和元素硫產率會較高。我們也發現觸媒若以CO和SO2同時進行預硫化，則其性能會高於以其它氣體 ( 如CO、SO2或He ) 進行預硫化處理。由SO2-TPD和CO-TPD的圖譜可以看出Cr2O3 /nano-CeO2觸媒比其它觸媒更容易吸附和脫附SO2 和CO，此結果可以適當地解釋Cr2O3 /nano-CeO2觸媒對於SO2 的還原反應有較高活性之原由。我們也對自己所研發之觸媒和先前已發表於期刊上所使用之觸媒，就它們的性能作了比較。

　　為了研發能同時處理二氧化硫及一氧化氮之觸媒，我們接著進行以金屬氧化物/nano-CeO2觸媒催化一氧化氮之還原反應。使用先前所製備之奈米級金屬氧化物/二氧化鈰擔體觸媒，進行以一氧化碳還原一氧化氮之還原反應，並對它們的性能進行評估。
對催化以一氧化碳為還原劑之一氧化氮還原反應，於奈米CeO2作為擔體之六種金屬氧化物擔體觸媒中，以NiO/CeO2觸媒具最佳活性，CuO/CeO2 觸媒次之。為了探討擔體效應，我們又以CeO2、γ-Al2O3及TiO2三種擔體製備NiO/擔體觸媒，活性測試結果顯示：以CeO2 為擔體者具最佳之活性，γ-Al2O3次之。改變NiO/CeO2 擔體觸媒中NiO的含量，我們發現當鎳含量為5 wt%時，分散度最佳，而且活性最高。為了更進一步解釋何以所製備之NiO/擔體觸媒中，以CeO2 為擔體者具最佳之活性。接著我們以XRD、BET、CO－TPR、CO－TPD及NO－TPD來對奈米級金屬氧化物擔體觸媒作鑑定分析。由CO－TPR圖譜中發現NiO/CeO2 擔體觸媒較NiO/γ-Al2O3 擔體觸媒容易被還原，此與一氧化氮還原反應之催化活性相互脗合 ( NiO/CeO2 > NiO/γ-Al2O3 )。由NO－TPD圖譜發現，NiO/CeO2 和NiO/γ-Al2O3 擔體觸媒對一氧化氮皆具有吸附和脫附能力。根據CO－TPD實驗結果，發現CO會與NiO/CeO2 擔體觸媒中之氧反應生成CO2；然而CO卻不會與NiO/γ-Al2O3 擔體觸媒中之氧反應生成CO2。綜合CO－TPR、NO－TPD及CO－TPD之結果，我們可以推測：在NiO/CeO2 觸媒上發生之以一氧化碳與一氧化氮之反應，包含兩個反應機構，亦即是依兩個反應機構同時進行。其一為Eley-Rideal反應機構，是NO先被吸附於活性基座上 ( 低於200 oC就可被吸附 )，再與氣相中之CO進行一氧化氮之還原反應。其二為Mars-Van Krevelen反應機構，CO先將觸媒還原成還原態，本身變成CO2 （此一反應在大約100 oC就可發生），隨後NO再將觸媒氧化成氧化態，本身則被還原形成N2；此氧化及還原反應交互發生。

　　最後對本論文作總結，也對未來研究方向提出建議。

　In this study, the catalytic reduction of sulfur dioxide and nitric oxide was investigated. We prepared and selected the high performance catalysts first, and then carried out physical characterization, kinetic studies, as well as TPR and TPD experiments. Basing on the experimental results, we evaluated the activity, selectivity and stability and figure out suitable reaction mechanisms for both SO2 and NO reduction reactions . In addition, the effects of pretreatment and adding water vapor and oxygen in the feed on the conversions, fractional yields and the stabilities of catalysts were also included in our research.

　In the work for the catalytic reduction of SO2 with H2 as a reducing agent, NiO/g-Al2O3 catalyst was found to be the most active catalyst among the seven g-Al2O3-supported metal-oxide catalysts tested. With NiO as the active species, of the supports tested, g-Al2O3 was the most suitable one and the optimal Ni content was 16 wt%. Using this NiO/g-Al2O3 catalyst, we found that the optimal feed ratio of H2/SO2 is 2:1 and the catalyst presulfided with H2+H2S exhibits a higher performance than that pretreated with H2 or He. XRD patterns reveal that the nickel oxide experienced a transformation to Ni3S2 and NiS, and then to NiS2, the most active nickel sulfide, during the reaction process.

　For the catalytic reduction of SO2 to elemental sulfur with CO as a reducing gas, nanosized CeO2 was first synthesized by sol-gel method and then used as the support to prepare six kinds of supported metal-oxide catalysts by incipient wetness impregnation method. The cause for different activities is also closely examined by characterizing the catalyst by TEM, SEM and XRD. The size of nanosized CeO2 particle synthesized by sol-gel method is about 20-50nm. Experimental results indicate that Cr2O3/nano-CeO2 was the most active catalyst. Using this catalyst, a kinetic study was performed on the reduction of SO2 and the optimal feed ratio of CO/SO2 was found to be 2.5/1, and low concentrations of SO2 and CO provide a high SO2 conversion and sulfur yield. It was also found that the catalyst presulfied by CO+SO2 exhibits a higher performance than those pretreated with CO, SO2 or He. The discrepancy in the stability and activity resulted in the pretreatment has been rationally explained. The temperature- programmed desorption patterns of SO2 and CO illustrate that Cr2O3/nano-CeO2 can adsorb and desorb SO2 and CO more easily than can other catalysts. These results may properly explain why Cr2O3/nano-CeO2 has a higher activity for the reduction of SO2. The catalyst we prepared is also compared with those reported in the literature basing on their activities and stabilities.

　For finding the best catalyst of simultaneous treatment for sulfur dioxide and nitric oxide. The performance of the supported metallic oxide catalysts for catalytic reduction of NO with CO as a reducing agent were investigated. NiO/CeO2 catalyst was found to be the most active catalyst among the six CeO2-supported metal-oxide catalysts tested. Furthermore, among the three supported NiO catalysts with CeO2, g-Al2O3 and TiO2 as the supports, the CeO2-supported NiO catalyst has the highest activity and g-Al2O3-supported one is the second. With NiO as the active species and CeO2 as the support, the optimal Ni content was 5 wt%. Subsequently, these prepared catalysts were characterized with XRD, BET, CO-TPR, CO-TPD and NO-TPD in order to understand the effects of the catalyst characters on the catalytic activities. The CO-TPR pattern also shows that the temperature range at which the CO reduction takes place on NiO/CeO2 catalyst is lower than that on NiO/g-Al2O3 catalyst. The NO-TPD experiments reveal that NO can be adsorbed and desorbed by both NiO/CeO2 catalyst and NiO/g-Al2O3 catalyst. The CO-TPD pattern also shows that the CO can react with the oxygen of the NiO/CeO2 catalyst to form CO2, but can not do the NiO/g-Al2O3 catalyst. The CO-TPR, NO-TPD and CO-TPD experiments reveal that the catalytic reduction of NO with CO includes two reaction mechanisms. One of them is the Eley Rideal mechanism, by which the NO molecule is adsorbed to the active site first (at a temperature lower than 200 oC ) and then reacts with CO molecule in the gas phase to form N2 and CO2； another is the Mars-Van Krevelen mechanism, by which the oxidized form of catalyst reacts with the CO molecule to form CO2 and itself transforms to the reduced form ( this reaction takes place at about 100 oC ), subsequently, the catalyst in the reduced form reacts with NO molecule to form N2 and itself transforms back to the oxidized form, and the above oxidation-reduction reactions ( redox reactions ) occur alternatively.

　At the end of this dissertation, some conclusions are drawn basing on the discussion in each chapter and some suggestions for the future studies are also included.

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