赤泥負載金屬氧化物催化劑的制備及其脫硝性能研究
發(fā)布時間:2018-05-30 23:28
本文選題:脫硝催化劑 + 氮氧化物 ; 參考:《濟南大學》2015年碩士論文
【摘要】:近年來,隨著工業(yè)和經濟的快速發(fā)展,大量燃料的燃燒及機動車尾氣的大量排放導致氮氧化物的危害日益嚴峻。氮氧化物(NOx)是造成酸雨、臭氧層破壞和光化學煙霧的主要污染物之一,對自然環(huán)境和人類健康都有著很大的危害。關于氮氧化物的去除,目前研究最廣泛也最有應用前景的是以NH3為還原劑選擇性催化還原(NH3-SCR)技術。而NH3-SCR技術的核心就是催化劑,應用最廣泛的就是V2O5-WO3/TiO2體系催化劑,該類催化劑雖然脫硝活性高,但該類催化劑存在活性溫度高、成本高,活性組分釩氧化物有劇毒等缺陷。赤泥作為鋁廠的工業(yè)廢渣,因具有強堿性其引起的環(huán)境污染問題不容忽視;诔嗄啾旧砗写罅康难趸F、氧化鋁、氧化硅、氧化鈦等組分,這些組分對脫硝都有一定的促進作用:其中鐵氧化物具有很好的催化脫硝活性,氧化鋁、氧化硅是被廣泛研究的脫硝催化劑的載體,因此赤泥為基礎制備脫硝催化劑的研究具有一定的可行性,作為脫硝催化劑的研究具有實際的應用意義。此外赤泥含有大量的堿性組分Na、Ca等,阻礙其工業(yè)化應用,因此還需要對赤泥進行一定的預處理方可實現(xiàn)其催化脫硝應用。本論文采用鋁廠工業(yè)廢渣赤泥為原料,經過預處理后負載金屬氧化物活性組分,制備了一系列赤泥脫硝催化劑。利用X射線粉末衍射(XRD)對赤泥的物相進行了確認,結果顯示赤泥中主要物種是Fe2O3、SiO2、TiO2、Al(OH)3等物種,通過X射線熒光光譜儀(XRF)進一步證明了赤泥中含有大量的Fe、Al、Si等的氧化物。對赤泥的預處理結果表明預處理不僅降低了赤泥堿含量,而且大大提高了赤泥的比表面積,改善了赤泥的孔結構,提高了脫硝活性。赤泥的預處理工藝簡單經濟,預處理赤泥在催化領域有很好的應用前景。向赤泥上負載不同金屬氧化物組分后,活性評價結果表明,相比Mo、Co、Ni的氧化物,V和Cu的氧化物負載的赤泥具有更高的脫硝活性。通過合成一系列不同負載量的V、Cu赤泥脫硝催化劑,考察了活性組分負載量對催化劑脫硝性能的影響,結果表明隨著活性組分的增加,催化劑脫硝性能呈現(xiàn)先升高再降低的趨勢,說明活性組分在赤泥表面上存在一個最佳負載比,這個比值隨載體和活性組分不同而有所不同。本文采用比表面積分析儀、掃描電子顯微鏡(SEM)、X射線衍射(XRD)等表征技術研究赤泥脫硝催化劑的形貌及微觀結構;利用H2程序升溫還原技術研究催化劑的氧化還原性能;結合NO-TPD和原位紅外的研究結果,分析探討了催化劑的性能與結構之間的關系。綜合上述性能測試結果,7Cu/PTRM催化劑的具有適宜的性能,展現(xiàn)出現(xiàn)有實驗條件下最好的催化活性。
[Abstract]:In recent years, with the rapid development of industry and economy, the combustion of a large amount of fuel and a large number of vehicle exhaust emissions lead to the increasingly serious harm of nitrogen oxides. Nitric oxide (NOX) is one of the main pollutants causing acid rain, ozone depletion and photochemical smog, which is harmful to natural environment and human health. As for the removal of nitrogen oxides, the technology of selective catalytic reduction of NH _ 3-SCR with NH3 as reducing agent is the most widely studied and most promising. The core of NH3-SCR technology is catalyst, and the most widely used catalyst is V2O5-WO3/TiO2 system catalyst. Although this kind of catalyst has high denitrification activity, but this kind of catalyst has the defects such as high activity temperature, high cost and so on, the active component vanadium oxide has the extremely toxic and so on. Red mud, as the industrial waste residue of aluminum plant, can not be ignored because of its strong alkalinity. Based on the fact that the red mud itself contains a lot of iron oxide, alumina, silicon oxide, titanium oxide and so on, these components can promote denitrification to a certain extent: iron oxides have good catalytic denitrification activity, alumina, Silicon oxide is a widely studied carrier of denitrification catalyst, so it is feasible to study the preparation of denitrification catalyst based on red mud, and the research as a denitrification catalyst has practical application significance. In addition, red mud contains a large amount of basic components, such as Na ~ (2 +) Ca, which hinders its industrial application. Therefore, it also needs some pretreatment to realize the application of catalytic denitrification of red mud. In this paper, a series of red mud denitrification catalysts were prepared by using red mud from industrial waste residue of aluminum plant as raw material and loading active components of metal oxides after pretreatment. The phase of red mud was confirmed by X-ray powder diffraction (XRD). The results showed that the main species in red mud were Fe2O3SiO2SiO2O2O2AlOOHHH3. The results of X-ray fluorescence spectrometer (XRF) further proved that the red mud contained a large amount of oxides such as Feo Al Si and so on. The pretreatment results showed that the pretreatment not only reduced the alkali content of red mud, but also greatly improved the specific surface area, pore structure and denitrification activity of red mud. The pretreatment process of red mud is simple and economical. After loading different metal oxides on the red mud, the results of activity evaluation showed that the red mud had higher denitrification activity than that of the red mud loaded with the oxides of Mo-Co-Ni and Cu. Through the synthesis of a series of VGU red mud denitrification catalysts with different loading amounts, the effect of the active component loading on the denitrification performance of the catalyst was investigated. The results showed that the denitrification performance of the catalyst increased first and then decreased with the increase of the active component. It is concluded that there is an optimum loading ratio of active components on the surface of red mud, which varies with the carrier and active components. In this paper, the morphology and microstructure of red mud denitrification catalyst were studied by means of specific surface area analyzer and scanning electron microscope (SEM), and the redox performance of the catalyst was studied by H 2 temperature programmed reduction technique. Based on the results of NO-TPD and in situ IR, the relationship between the performance and structure of the catalyst was analyzed and discussed. The results show that the 7Cu / PTRM catalyst has the best catalytic activity under the experimental conditions.
【學位授予單位】:濟南大學
【學位級別】:碩士
【學位授予年份】:2015
【分類號】:O643.36;X701
【參考文獻】
相關期刊論文 前1條
1 苗繼斌;錢家盛;章于川;;十八烷基三甲基溴化銨為模板合成有序介孔氧化硅及其表征[J];中國粉體技術;2008年03期
,本文編號:1957305
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