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銅錳鈰三元催化劑的制備及其催化燃燒甲苯性能的研究

發(fā)布時(shí)間:2018-03-04 20:01

  本文選題:銅錳鈰 切入點(diǎn):負(fù)載量 出處:《浙江工業(yè)大學(xué)》2016年碩士論文 論文類型:學(xué)位論文


【摘要】:鑒于貴金屬過高的成本,銅錳氧化物作為常見的過渡金屬氧化物常被用于催化氧化有機(jī)揮發(fā)性污染物(VOCs)。CeO_2具有較好的儲氧功能,常與銅錳氧化物形成二元或三元催化劑來提高催化劑的催化性能。本論文中,采用浸漬法制備了以TiO_2為載體的銅錳二元復(fù)合氧化物催化劑和銅錳鈰三元復(fù)合氧化物催化劑。通過XRD、BET和H2-TPR表征技術(shù)考察了Cu/Mn摩爾比及負(fù)載量、Cu/Mn/Ce摩爾比及負(fù)載量對催化劑晶相結(jié)構(gòu)和氧流動性的影響。然后,采用溶膠凝膠法制備了銅錳鈰三元復(fù)合氧化物催化劑,通過XRD、BET和H2-TPR表征技術(shù)考察了焙燒溫度對催化劑晶相結(jié)構(gòu)和氧流動性的影響。并采用常壓氣-固反應(yīng)裝置以甲苯作為探針反應(yīng),評價(jià)催化劑催化燃燒甲苯的性能和穩(wěn)定性。得到的結(jié)果如下所示:1.采用浸漬法制備的Cu-Mn/TiO_2催化劑在焙燒溫度為500℃時(shí)通過固相反應(yīng)生成了復(fù)合氧化物Cu1.4Mn1.6O4。在復(fù)合氧化物Cu1.4Mn1.6O4中,銅錳之間的協(xié)同作用提高了催化劑的催化氧化性能。當(dāng)Cu/Mn摩爾比為1:1、負(fù)載量為30%時(shí),銅錳二元氧化物催化劑的催化性能最佳,其T95為277.5℃。2.采用浸漬法制備Cu/Mn/Ce摩爾比為1:1:4、負(fù)載量為30%的銅錳鈰三元氧化物催化劑催化性能最佳,其T95為274.7℃。CeO_2的加入可以提高Cu1.4Mn1.6O4的分散度,提高了氧的流動性,從而降低了催化劑的H2-TPR還原峰溫。進(jìn)而提高了催化劑的催化氧化性能。且催化劑有很好的穩(wěn)定性,在275℃下反應(yīng)30天,轉(zhuǎn)化率和選擇性不變。3.與浸漬法制備的負(fù)載型銅錳鈰氧化物催化劑(負(fù)載量為30%、摩爾比為1:1:4)相比,溶膠凝膠法制備的銅錳鈰三元復(fù)合氧化物催化劑(摩爾比為1:1:4、焙燒溫度為500℃)催化性能更佳,其T95為236.2℃。主要由于溶膠凝膠法制備的不加載體的催化劑活性組分具有更大的比表面積,活性中心(CuO,Cu1.4Mn1.6O4等)分散度更高,形成的活性位點(diǎn)更多,從而提高了催化劑催化氧化甲苯的性能。此外,催化劑有很好的穩(wěn)定性,在236℃下反應(yīng)30天,轉(zhuǎn)化率和選擇性基本不變。
[Abstract]:In view of the high cost of precious metals, Cu-Mn oxides, as common transition metal oxides, are often used to catalyze the oxidation of volatile organic pollutants (VOCsN). CeOSP _ 2 has a better oxygen storage function. Binary or ternary catalysts are often formed with Cu-Mn oxides to improve the catalytic performance of the catalysts. The copper-manganese binary oxide catalysts and copper-manganese cerium ternary oxide catalysts supported on TiO_2 were prepared by impregnation method. The molar ratio of Cu/Mn and the amount of supported Cu / mn / ce were investigated by XRDX BET and H2-TPR characterization techniques. Effect of catalyst phase structure and oxygen fluidity. Then, The copper-manganese and cerium ternary oxide catalysts were prepared by sol-gel method. The effects of calcination temperature on the crystal structure and oxygen fluidity of the catalyst were investigated by means of XRDX BET and H2-TPR characterization techniques, and toluene was used as a probe in the atmospheric pressure gas-solid reactor. The performance and stability of catalyst for toluene combustion were evaluated. The results are as follows: 1. The Cu-Mn/TiO_2 catalyst prepared by impregnation method has been prepared by solid state reaction at 500 鈩,

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