金屬絲網(wǎng)蜂窩催化劑的制備及應(yīng)用

【中文摘要】 金屬絲網(wǎng)蜂窩催化劑是以成型金屬絲網(wǎng)為支撐體的新型結(jié)構(gòu)化催化材料。由于其主通道壁是通透的絲網(wǎng),網(wǎng)孔為流體徑向混合提供了旁路,能明顯改善流體分布、混合狀況,提高傳遞效率。本論文以開發(fā)通用型的金屬絲網(wǎng)蜂窩催化劑為目標(biāo),研究制備中的關(guān)鍵問題。在此基礎(chǔ)上,試制了涂覆有Pd/Al2O3活性成分的金屬絲網(wǎng)蜂窩催化劑,并以甲烷催化燃燒體系為例,與陶瓷支撐體蜂窩催化劑的反應(yīng)結(jié)果進(jìn)行對(duì)比驗(yàn)證。催化層與金屬支撐體結(jié)合的牢固性是金屬絲網(wǎng)蜂窩催化劑開發(fā)中的關(guān)鍵難題。本課題采用電泳沉積法在支撐體上制備鋁/氧化鋁復(fù)合層作為催化層與支撐體之間的過渡層�？疾炝艘掖肌⒍⊥�、丙酮三類懸浮液體系中各操作參數(shù)對(duì)電泳沉積結(jié)果的影響,找出了制備均勻涂層的適宜條件。即在乙醇體系中為PVP:0.2wt.%、三氯化鋁:2.5mM、鋁粉:1wt.%、電場(chǎng)強(qiáng)度:30V/cm、沉積時(shí)間:10min;丁酮體系中為硝化纖維:0.6wt.%、正丁胺:10vol.%、鋁粉:0.2wt.%、電場(chǎng)強(qiáng)度:50V/cm、沉積時(shí)間:30min;丙酮體系中為丙酮:50mL、硝化纖維:0.1g、鋁粉:1g、四甲基氫氧化銨:0.3mg、磷酸:0.25mg、電場(chǎng)強(qiáng)度:25 V/cm、沉積時(shí)間:3min。相較于乙醇、丁酮體系,丙酮懸浮液體系更加穩(wěn)定,所得涂層初強(qiáng)度高,涂層厚度為50μm,適宜整體金屬絲網(wǎng)的電泳沉積。將丙酮體系電泳沉積所得鋁顆粒涂層進(jìn)行氮?dú)獗Ｗo(hù)下的高溫?zé)崽幚砗偷蜐舛劝彼�處理得到結(jié)合牢固,比表面積大的鋁/三氧化二鋁載體層。金屬絲網(wǎng)經(jīng)過電泳沉積、高溫?zé)崽幚�、化學(xué)處理和整體成型后,得到直徑25 mm,高度21mm,重量10 g,幾何面積37.1cm2/g的金屬蜂窩絲網(wǎng)催化劑載體。將該載體涂覆Pb/Al2O3粉末催化劑(粉末中Pb負(fù)載量為0.33 wt.%)(催化劑中Pb負(fù)載量為0.103 wt.%),在甲烷催化燃燒反應(yīng)中進(jìn)行考評(píng)。該催化劑的催化活性高于陶瓷蜂窩催化劑,反應(yīng)溫度為600℃時(shí),甲烷轉(zhuǎn)化率比陶瓷蜂窩催化劑的高10.89%,宏觀反應(yīng)速率常數(shù)是后者的2.18倍
【英文摘要】 Wire-mesh honeycomb (WMH) is a category of novel monolithic catalysts supported on structured wire-mesh substrate. As the conduct of WMH is made of mesh, whose pores provide fluids the bypass of radical mixing across the bed diameter, which effect can improve the fluid distribution and mixing state, thus raises transfer efficiency. Aimed at developing a WMH for general applications, this thesis tried to breakthrough the key difficulties in WMH preparation. For purpose of demonstration, the WMH washcoated by Pd/Al2O3 was prepared and applied in catalytic combustion of air diluted methane, with its result compared to the ceramic counterpart.The key problem in developing WHM is the fast adhesion of the active catalyst powder with the metallic mesh. To solve this problem, an aluminum/alumina coating was prepared by electrophoretic deposition (EPD) on top of wire-mesh surface. Experiments were carried out to find the optimal conditions in ethanol, butanone and acetone suspension for depositing a uniform Al particulate coating, which are concluded as below: in ethanol suspension, PVP: 0.2 wt.%, AlCl3: 2.5 mM, Al powder: 1wt.%, electric field intensity: 30 V/cm, deposition time: 10min; in butanone suspension, nitrocellulose: 0.6 wt.%, n-butylamine: 10 vol.%, Al powder: 0.2 wt.%, electrical field intensity: 50 V/cm, deposition time: 30 min, while in acetone suspension, acetone: 50 mL, nitrocellulose: 0.1 g, Al powder: 1 g, teramethyl ammonium hydroxide: 0.3 mg, phosphoric acid: 0.25 mg, electrical field intensity: 25 V/cm, deposition time: 3 min. Acetone suspension is more stable and the adherence of deposited coatings are higher than ethanol and butanone suspension, and the coating thickness is 50μm. Well adherent and porous aluminum/alumina top layers were prepared by thermal and chemical treatment of the deposited coatings in acetone suspension.After EPD, thermal & chemical treatment, and mould processing, the WMH support was prepared, which was 25 mm in diameter, 21 mm in height, 10 g in weight and 37.1 cm2/g in geometric surface area. The WMH catalyst washcoated with Pb/Al2O3 (Pb wt.% = 0.33%) was tested in catalytic combustion of air diluted methane. Compared at 600℃, CH4 conversion in WMH is 10.89% higher than the catalyst supported on ceramic substrate and the overall reaction rate constant more than doubled.

【中文關(guān)鍵詞】 金屬絲網(wǎng)蜂窩催化劑; 電泳沉積; 熱處理; 化學(xué)處理; 甲烷催化燃燒
【英文關(guān)鍵詞】 wire-mesh honeycomb catalyst; electrophoretic deposition; thermal treatment; chemical treatment; catalytic combustion of methane
【畢業(yè)論文目錄】
摘要 4-6
ABSTRACT 6-7
第一章 緒論 10-28
    1.1 研究背景 10-11
    1.2 整體式催化劑 11-17
        1.2.1 整體式催化劑組成 11-13
        1.2.2 整體式催化劑特點(diǎn) 13-14
        1.2.3 整體式催化劑研究與進(jìn)展 14-15
        1.2.4 整體式催化劑應(yīng)用前景 15-17 
    1.3 金屬載體催化劑涂層制備技術(shù) 17-25
        1.3.1 金屬載體催化劑涂層制備方法 17-20
        1.3.2 電泳沉積法簡(jiǎn)述 20-25
    1.4 甲烷催化燃燒簡(jiǎn)介 25-26
    1.5 本論文主要研究?jī)?nèi)容 26-28
第二章 電泳沉積法在FeCrAl 合金絲網(wǎng)上制備鋁顆粒涂層 28-47
    2.1 實(shí)驗(yàn)部分 28-31
        2.1.1 FeCrAl 金屬絲網(wǎng)支撐體的預(yù)處理 28
        2.1.2 鋁粉的預(yù)處理 28
        2.1.3 乙醇體系中電泳沉積法制備鋁顆粒涂層 28-30
        2.1.4 丁酮體系中電泳沉積法制備鋁顆粒涂層 30
        2.1.5 丙酮體系中電泳沉積法制備鋁顆粒涂層 30-31
    2.2 結(jié)果與討論 31-45
        2.2.1 FeCrAl 合金絲網(wǎng)和鋁粉預(yù)處理結(jié)果分析 31-32
        2.2.2 乙醇體系中鋁顆粒電泳沉積的結(jié)果討論 32-37
        2.2.3 丁酮體系中鋁顆粒電泳沉積的結(jié)果討論 37-40
        2.2.4 丙酮體系中鋁顆粒電泳沉積的結(jié)果討論 40-45
    2.3 本章小結(jié) 45-47
第三章 鋁顆粒涂層的后處理及金屬蜂窩載體的成型 47-54
    3.1 實(shí)驗(yàn)部分 47-49
        3.1.1 鋁顆粒涂層的熱處理 47
        3.1.2 鋁顆粒涂層的化學(xué)處理 47-48
        3.1.3 FeCrAl 金屬絲網(wǎng)蜂窩載體的制備 48-49
    3.2 結(jié)果與討論 49-53
        3.2.1 鋁顆粒涂層的熱處理 49-51
        3.2.2 鋁顆粒涂層的化學(xué)處理 51-52
        3.2.3 FeCrAl 金屬絲網(wǎng)蜂窩載體 52-53
    3.3 本章小結(jié) 53-54
第四章 FeCrAl 金屬絲網(wǎng)蜂窩催化劑在甲烷催化燃燒中的應(yīng)用 54-59
    4.1 實(shí)驗(yàn)部分 54-55
        4.1.1 實(shí)驗(yàn)?zāi)康?54
        4.1.2 實(shí)驗(yàn)儀器與試劑 54-55
        4.1.3 實(shí)驗(yàn)步驟 55
    4.2 結(jié)果與討論 55-58
        4.2.1 載體催化活性組分的涂敷 55-56
        4.2.2 金屬絲網(wǎng)和氧化鋁陶瓷催化劑活性及反應(yīng)速率常數(shù)對(duì)比 56-58
    4.3 本章小結(jié) 58-59
第五章 全文總結(jié) 59-62
    5.1 主要結(jié)論 59-61
    5.2 研究展望 61-62
參考文獻(xiàn) 62-66
致謝 66-67
攻讀碩士學(xué)位期間發(fā)表的論文 67-68
上海交通大學(xué)學(xué)位論文答辯決議書 68

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