本文選題：室溫固相反應(yīng) + 高能球磨法�。� 參考：《復(fù)旦大學(xué)》2011年碩士論文

【摘要】：隨著政府、社會(huì)和公眾對(duì)環(huán)境保護(hù)的要求越來越高,如何處理工業(yè)生產(chǎn)尾氣中的揮發(fā)性有機(jī)物(VOCs)成為環(huán)保方面研究的熱點(diǎn)。催化燃燒技術(shù)作為最有效的處理有機(jī)廢氣的方法受到了研究者的重視,開發(fā)高效、廉價(jià)催化劑是相關(guān)研究亟待解決的一個(gè)問題。貴金屬催化劑雖然活性好,但是高昂的價(jià)格大大限制了它的應(yīng)用,過渡金屬氧化物催化劑作為貴金屬催化劑的替代物引起了大家的關(guān)注。本文從改進(jìn)催化劑制備方法以提高催化劑活性的角度出發(fā),研究了簡(jiǎn)單、高效、低能耗的固相法在氧化物催化劑的制備中的應(yīng)用,我們通過室溫固相法制備了Co3O4、CeO2、Mn2O3,通過高能球磨法制備制備了銅鈷復(fù)合氧化物,在催化甲苯完全氧化時(shí)均表現(xiàn)出很好的活性。具體如下：1、固相法制備四氧化鈷催化劑及其催化甲苯完全氧化Co3O4是被廣泛應(yīng)用的催化劑,在催化氧化、電化學(xué)、傳感器等方面有重要的應(yīng)用。我們采用室溫固相反應(yīng)制備了Co3O4的前驅(qū)體,經(jīng)過一定溫度的焙燒,得到了納米Co3O4,本方法過程簡(jiǎn)單,能耗低,環(huán)境友好。與常規(guī)的沉淀法、檸檬酸絡(luò)合-燃燒法相比,固相法制備得到的Co3O4催化劑粒徑小、表面缺陷較多、表面Co-O鍵較弱、表面吸附氧豐富,具有更好的活化氧的能力,表現(xiàn)出更好的催化甲苯完全氧化活性。催化劑前驅(qū)體的焙燒溫度對(duì)催化劑的活性有很大影響,400℃C焙燒時(shí)催化劑的性能最優(yōu)。對(duì)催化劑進(jìn)行了60小時(shí)的老化測(cè)試,在230℃甲苯的轉(zhuǎn)化率始終保持在95%以上。2、固相法制備氧化鈰催化劑及其催化甲苯完全氧化氧化鈰在催化中有非常廣泛的應(yīng)用,既可以作為催化劑助劑,也可以作為主要的活性組分,還是很好的催化劑載體。我們采用固相法制備的納米氧化鈰在催化甲苯的完全氧化反應(yīng)中表現(xiàn)出了非常好的活性,BET、XRD、Raman、SEM、H2-TPR等表征表明,固相法制備得到的Ce02催化劑粒徑小、表面缺陷較多、表面吸附氧豐富,活化氧的能力強(qiáng)。前驅(qū)體的焙燒溫度對(duì)催化劑的活性有很大影響,500℃焙燒時(shí)催化劑的性能最優(yōu)。對(duì)催化劑進(jìn)行的100小時(shí)的老化表明,在215℃C甲苯的轉(zhuǎn)化率始終保持在95%以上。3、固相法制備氧化錳催化劑及其催化甲苯完全氧化我們采用與前面相同的固相法制備得到了Mn203催化劑,與檸檬酸絡(luò)合-燃燒法和沉淀法制備的錳氧化物相比,固相法制備得到的Mn203催化劑粒徑小、表面缺陷較多、低溫氧化還原性能好,具有更好的活化氧的能力,所以催化甲苯完全氧化的能力更強(qiáng)。同時(shí),催化劑前驅(qū)體的焙燒溫度對(duì)錳催化劑的活性有很大影響,3500C焙燒時(shí)催化劑的性能最優(yōu),同時(shí)前驅(qū)體已經(jīng)分解完全,在246℃就可以達(dá)到95%的甲苯轉(zhuǎn)化率。4、高能球磨法制備銅鈷復(fù)合氧化物及其催化甲苯完全氧化高能球磨法利用球磨機(jī)的高速震動(dòng)和轉(zhuǎn)動(dòng)使硬球?qū)υ线M(jìn)行強(qiáng)烈的撞擊、研磨和攪拌,從而使粉末顆粒產(chǎn)生塑性形變、顆粒內(nèi)產(chǎn)生大量的缺陷,在顆粒的接觸面達(dá)到局部高溫誘發(fā)化學(xué)反應(yīng)發(fā)生,這樣得到的復(fù)合氧化物即處于納米范疇之內(nèi),同時(shí)又在表面富集有很多缺陷位,為反應(yīng)提供了活性中心。我們通過高能球磨法制備得到銅鈷復(fù)合氧化物催化劑,與傳統(tǒng)的共沉淀法相比,高能球磨法制備的催化劑活性更好,6小時(shí)碾磨制備的催化劑,在2220C時(shí)甲苯的轉(zhuǎn)化率就可以達(dá)到50%,230℃時(shí)甲苯的轉(zhuǎn)化率超過95%。通過表征表明高能球磨法制備的催化劑晶粒較小、表面缺陷豐富,這都有利于甲苯的完全氧化的反應(yīng)。穩(wěn)定性測(cè)試表明,固相法制備的催化劑的抗老化能力也更強(qiáng)。
[Abstract]:With the government, society and the public are becoming more and more demanding for environmental protection, how to deal with volatile organic compounds (VOCs) in industrial production exhaust has become a hot topic in environmental protection research. As the most effective method of treating organic waste gas, catalytic combustion technology has been re viewed by researchers. It is urgent to develop high efficiency and cheap catalysts. A solution to the problem. Although the noble metal catalyst has good activity, the high price greatly restricts its application. The transition metal oxide catalyst as a substitute for the noble metal catalyst has aroused the attention of everyone. This paper is simple, efficient and low in the view of improving the catalyst preparation method to improve the activity of the catalyst. The application of energy consumption solid phase method in the preparation of oxide catalysts, Co3O4, CeO2, Mn2O3 were prepared by solid-state method at room temperature. The co oxides of copper and cobalt were prepared by high energy ball milling, and they all showed good activity during the complete oxidation of toluene. 1, the solid phase method was used to prepare cobalt four catalyst and its catalytic armor. Benzene complete oxidation Co3O4 is a widely used catalyst. It has important applications in catalytic oxidation, electrochemistry, sensor and so on. We prepared the precursor of Co3O4 by solid state reaction at room temperature. After a certain temperature roasting, the nano Co3O4 was obtained. The process is simple, energy consumption is low, and the environment is friendly. Compared with the combined combustion method, the Co3O4 catalyst prepared by the solid-phase method has small particle size, more surface defects, weak surface Co-O bond, rich oxygen adsorption on the surface, better ability of activating oxygen, and better catalytic activity of toluene. The calcination temperature of the precursor catalyst has a great influence on the activity of the catalyst, when the catalyst is calcined at 400 C for C The performance of the catalyst is the best. The catalyst has been tested for 60 hours, and the conversion rate of toluene at 230 centigrade remains above 95%.2. The solid phase preparation of cerium oxide catalyst and its catalytic toluene oxide fully oxidize cerium oxide are widely used in the catalysis. It can be used as a catalyst agent and as the main active group. BET, XRD, Raman, SEM, H2-TPR and so on showed that the particle size of the Ce02 catalyst prepared by the solid phase method was small, the surface defects were more, the surface adsorbed oxygen was abundant and the ability of activating oxygen was strong. The calcination temperature of the precursor has a great influence on the activity of the catalyst, and the performance of the catalyst is the best when roasting at 500 C. The 100 hour aging of the catalyst shows that the conversion rate of toluene at 215 C is kept above 95%. The solid phase method for the preparation of manganese oxide catalyst and the complete oxidation of toluene we use the same solid as in front of the catalyst. The Mn203 catalyst was prepared by phase method. Compared with the manganese oxides prepared by the citric acid complex combustion method and the precipitation method, the Mn203 catalyst prepared by the solid phase method has small particle size, more surface defects, better oxidation reduction performance at low temperature and better ability of activating oxygen, so the ability to oxidize toluene to complete oxidation is stronger. At the same time, before the catalyst, the catalyst is more effective. The calcination temperature of the drive has a great influence on the activity of the manganese catalyst. At the same time, the performance of the catalyst is the best when 3500C is roasted. At the same time, the precursor has been completely decomposed, and the conversion rate of toluene can be up to 95% at 246 degrees C. The high energy ball milling method is used to prepare the copper cobalt complex oxide and the high velocity vibration of the complete oxidation of toluene by high energy ball milling. The hard ball has a strong impact on the raw material, grinding and stirring, so that the powder particles are plastic deformation, a large number of defects are produced in the particles, and the chemical reaction occurs in the contact surface of the particles. The compound oxide is in the nanometer category, and there are many defects on the surface. The catalyst was prepared by high energy ball milling. Compared with the traditional coprecipitation method, the activity of the catalyst prepared by high energy ball milling was better than that of the traditional co precipitation method. The conversion rate of toluene could reach 50% at 2220C and the conversion of toluene at 230 C was more than 95%. at 2220C. The results show that the catalysts prepared by high energy ball milling are small in grain and rich in surface defects, which are beneficial to the complete oxidation of toluene. The stability test shows that the anti-aging ability of the catalyst prepared by the solid phase method is also stronger.
【學(xué)位授予單位】：復(fù)旦大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2011
【分類號(hào)】：O643.364

【參考文獻(xiàn)】

相關(guān)期刊論文 前5條

1 徐金光,田志堅(jiān),王軍威,徐云鵬,徐竹生,林勵(lì)吾;CeO_2/BaMnAl_(11)O_(19-α)催化劑制備及甲烷催化燃燒研究[J];化學(xué)學(xué)報(bào);2004年04期

2 秦朝遠(yuǎn);喬彤森;;生物法處理氣體中易揮發(fā)性有機(jī)物研究進(jìn)展[J];石化技術(shù)與應(yīng)用;2006年01期

3 曹耀華,楊紹文,金梅,胡宏杰,趙恒勤;納米二氧化鈦降解有機(jī)污染物的試驗(yàn)研究[J];礦產(chǎn)保護(hù)與利用;2002年03期

4 楊_g,賈殿贈(zèng),葛煒煒,金春飛,忻新泉;低熱固相反應(yīng)制備無機(jī)納米材料的方法[J];無機(jī)化學(xué)學(xué)報(bào);2004年08期

5 王紅娟,李忠;半導(dǎo)體多相光催化氧化技術(shù)[J];現(xiàn)代化工;2002年02期

相關(guān)博士學(xué)位論文 前1條

1 賈殿贈(zèng);一維納米材料的低熱固相自組裝及機(jī)理研究[D];四川大學(xué);2005年

，

本文編號(hào)：2036898