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Dry reforming of methane using Ni-Ce catalysts supported on a modified mineral clay

机译:使用负载在改性矿物粘土上的Ni-Ce催化剂对甲烷进行干法重整

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Ni-Ce catalysts supported on mineral clay modified with Al and PVA (polyvinylic alcohol) were synthesized in the presence of microwave radiation. The effect of the nominal quantity of Ce (3,5 and 10wt.%) was analyzed. The catalysts calcined at 800 °C were characterized by elemental chemical analysis, XRD. TPR-H2, TPO and TEM, and evaluated in the reaction of CO2 reforming of methane between 500 and 800 °C, using a mixture of reacting agents of 5/5/40 CH4/CO2/Ar (50mL min~(-1)) without reduction pre-treatment. The XRD showed that the structure of the catalyst is thermally stable while the TPR-H2 suggested the formation of two types of main reducible species that are related with the different environments that Ni may adopt on the surface of the support. The catalysts showed high catalytic activities during two temperature cycles (increase and decrease) and high yields towards CO and H2 with molar ratios between 0.6 and 1.2. The active phase of the catalyst is stable under the conditions of the reaction since sintering was not observed. Ce showed a beneficial effect on the activities and catalytic selectivities of the solids and in the diminution of the production of coke, depending on the nominal quantity. With the increment of the quantity of Ce an increment in the conversions and catalytic selectivities was obtained. The catalyst with 3 wt.%. of Ce showed the lowest levels of coke production. After the catalytic process the main formation of nanotubes of coke on the surface of the catalyst was established.
机译:在微波辐射存在下,合成了负载有Al和PVA(聚乙烯醇)改性的矿物粘土的Ni-Ce催化剂。分析了铈的名义量(3.5和10wt。%)的影响。通过元素化学分析XRD对在800°C下煅烧的催化剂进行了表征。 TPR-H2,TPO和TEM,并使用5/5/40 CH4 / CO2 / Ar(50mL min〜(-1))反应混合物在500至800°C的甲烷CO2重整反应中进行评估),无需还原预处理。 XRD表明催化剂的结构是热稳定的,而TPR-H2表明形成了两种类型的主要可还原物种,它们与Ni可能在载体表面上采用的不同环境有关。催化剂在两个温度循环(升高和降低)中表现出高催化活性,摩尔比在0.6至1.2之间,对CO和H2的产率高。由于未观察到烧结,因此催化剂的活性相在反应条件下是稳定的。 Ce取决于标称量,对固体的活性和催化选择性以及焦炭产量的减少显示出有益的影响。随着Ce量的增加,获得转化率和催化选择性的增加。该催化剂具有3重量%。 Ce的焦炭产量最低。在催化过程之后,建立了在催化剂表面上焦炭纳米管的主要形成。

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