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Study on copper incorporated mesoporous silica SBA-15 for N2O catalytic decomposition

机译:含铜介孔二氧化硅SBA-15用于N2O催化分解的研究

摘要

Nitrous oxide (N20) is an environmental pollutant because it is a relatively strong greenhouse effect gas and contributes towards the destruction of ozone in theudstratosphere. Direct decomposition of N20 by catalysts represents one of the potential solutions to minimize N20 emissions. This research, focuses on Cu incorporation into SBA-15 mesoporous silica by pH modification method using hexamethylenetetrarnine (HMTA) as an internal pH-modifier and its potential use as a catalyst for N20uddecomposition. The effect of acidity on SBA-15 preparation through different initial HC1 concentration and the addition of HMTA as pH modifier were investigated. The SBA-15 formed well-ordered hexagonal mesoporous structure at high acidity (2.0 M) and poor ordered hexagonal pore structure at low acidity condition (0.005 M). It was found that under moderate acidic condition (0.1 M HC1) with addition of HMTA (HMTA:Si molar ratio 1:10), well-ordered hexagonal mesoporous SBA-15 could be produced. Meanwhile, copper was chosen for further studies on metal incorporation of SBA-15 (M/SBA-15) because Cu-containing SBA-15 has the highest catalytic activity for N20 decomposition compared to that of other first row transition metals impregnated on SBA-15. Copper incorporated mesoporous silica (Cu-SBA-15) has been successfully prepared by direct synthesis under medium acidic condition with addition of HMTA as a pH modifier. The Cu/SBA-15 produced were characterised using XRD, N2 adsorption-desorption, TEM, SEM, FT-IR, UV-vi, XPS and TPR. The results indicate that Cu was mainly incorporated into the framework of SBA- 15. The unit-cell, surface area, pore volume and wall thickness increased after the incorporation of the copper ions in SBA-15. HMTA plays a very important role to increase internal pH in order to introduce copper into the framework of SBA- 15 silica. Cu loading on Cu/SBA-ud15 determined using AAS is almost the same to the initial Cu amount, when the pH value is above isoelectronic of silica (pH=2) due to addition of HMTA. Higher amountudof HMTA, however, lead to the destruction of SBA-15 structure. Compared with Cu/SBA-15 impregnation method, Cu/SBA-15 prepared through pH modification method shows much higher activity for N20 catalytic decomposition due to 80% N20 conversion at 550 °C and reached 100% at 600 °C. The activation energy for the reaction catalysed by Cu/SBA-15 prepared through pH modification method is 91.9 -121.6 kJ/mol. This is much lower compared to that catalysed by CU/SBA-15 prepared though impregnation, that is in the range between 148.5 - 173.9 kJ/mol. Cu/SBA-15udincorporated sample also has higher activity due catalytic activity started at 300 °C and reaches more 80% conversion at 500 °C for catalytic reduction of N 20 by CH4.
机译:一氧化二氮(N20)是一种环境污染物,因为它是一种相对较强的温室效应气体,并且有助于破坏平流层中的臭氧。催化剂直接分解N2O是将N2O排放降至最低的潜在解决方案之一。这项研究的重点是通过使用六亚甲基四胺(HMTA)作为内部pH调节剂的pH调节方法将铜掺入SBA-15介孔二氧化硅中,以及将其潜在地用作N20 分解的催化剂。研究了酸度通过不同初始HCl浓度和添加HMTA作为pH调节剂对SBA-15制备的影响。 SBA-15在高酸度(2.0 M)下形成有序的六角形介孔结构,而在低酸度条件下(0.005 M)形成差的有序六边形孔结构。发现在中等酸性条件下(0.1 M HCl)添加HMTA(HMTA:Si摩尔比为1:10),可以生产出有序的六角形介孔SBA-15。同时,选择铜用于进一步研究SBA-15(M / SBA-15)的金属掺入情况,因为与浸渍在SBA-15上的其他第一行过渡金属相比,含Cu的SBA-15具有最高的N20分解催化活性。 15通过在中等酸性条件下直接合成并添加HMTA作为pH调节剂,已成功制备了含铜的介孔二氧化硅(Cu-SBA-15)。使用XRD,N2吸附-脱附,TEM,SEM,FT-IR,UV-vi,XPS和TPR对生成的Cu / SBA-15进行表征。结果表明,Cu主要被掺入SBA-15的骨架中。在SBA-15中掺入铜离子后,晶胞,表面积,孔体积和壁厚增加。 HMTA在增加内部pH值方面起着非常重要的作用,以便将铜引入SBA-15二氧化硅的骨架中。当由于添加HMTA而使pH值高于二氧化硅的等电子值(pH = 2)时,使用AAS测定的Cu / SBA-ud15上的Cu含量与初始Cu量几乎相同。然而,较高的HMTA含量会导致SBA-15结构的破坏。与Cu / SBA-15浸渍法相比,通过pH修饰法制备的Cu / SBA-15在550°C时有80%的N20转化率,在600°C时达到了100%,显示出更高的N20催化分解活性。 pH修饰法制得的Cu / SBA-15催化的反应活化能为91.9 -121.6 kJ / mol。与通过浸渍制备的CU / SBA-15催化的相比,它低得多,在148.5-173.9kJ / mol之间。 Cu / SBA-15 ud掺入的样品也具有较高的活性,这是由于从300°C开始的催化活性,并在500°C达到80%以上的转化率,以实现CH 4对N 20的催化还原。

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    Mohd Haizal Mohd Husin;

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  • 年度 2016
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