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Lanthanum-Doped Ceria Nanocomposite: A Highly Stable Monolithic Catalyst for Direct Synthesis of Dimethyl Carbonate

机译:镧系掺杂的二氧化铈纳米复合材料:一种高度稳定的整体催化剂,用于直接合成碳酸二甲酯

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That dimethyl carbonate is directly synthesized from methanol and carbon dioxide is an effective and environmental approach to solve the greenhouse effect. For the sake of solving the problems of low DMC productivity and poor catalysts stability in presence of the formed water. Here we design and prepare a serial of spherical La-doped ceria nanoparticles (Ce_(1-x)La_xO_ nanocomposites, x=0.00, 0.05, 0.10, 0.15, and 0.20) via a co-precipitation method. These Ce_(1-x)La_xO_ composites are ground into slurry by ball milled and then coated on cordierite honeycomb ceramics to obtain Ce_(1-x)La_xO_ monolithic catalysts. These Ce_(1-x)La_xO_ composites are characterized extensively by TEM, XRD, Raman spectroscopy, N_2 adsorption-desorption isotherms, H_2-TPR and XPS. The characterization results show that the Ce_(1-x)La_xO_ composites nanoparticles possesses richer surface oxygen vacancies, higher BET surface area and smaller particle size than that of pure CeO_2 nanoparticle. Besides, catalytic activity test shows these Ce_(1-x)La_xO_ monolithic catalysts exhibit better catalytic performance than that of pure CeO_2 nanoparticles. Among them, Ce_(0.95)La_(0.05)O_ monolithic catalyst exhibits the highest CH3OH conversion and DMC yield, which is in good line with the oxygen vacancy content measured by XPS. Finally, the Ce_(0.95)La_(0.05)O_ monolithic catalyst also shows an excellent durability of more than 100 hours, which is mainly due to the doping effect of lanthanum into the ceria oxides tailoring the structure and surface properties of the catalyst.
机译:碳酸二甲酯由甲醇直接合成,二氧化碳是解决温室效应的有效和环境的方法。为了解决所形成的水存在低DMC生产率和差催化剂稳定性的问题。在这里,我们通过共沉淀法设计和制备一系列球形La-掺杂的二氧化铈纳米颗粒(Ce_(1-x)La_xO_纳米复合材料,x = 0.00,0.05,0.10,0.15和0.20)。将这些CE_(1-x)LA_XO_复合材料通过球研磨成浆料,然后涂在堇青石蜂窝陶瓷上,得到CE_(1-x)LA_XO_单片催化剂。这些CE_(1-x)LA_XO_复合材料由TEM,XRD,拉曼光谱,N_2吸附 - 解吸等温,H_2-TPR和XPS进行了广泛的特征。表征结果表明CE_(1-X)LA_XO_复合材料纳米颗粒具有更丰富的表面氧空位,更高的BET表面积和比纯CEO_2纳米颗粒更小的粒度。此外,催化活性试验表明这些CE_(1-X)LA_XO_单片催化剂表现出比纯CeO_2纳米颗粒的催化性能更好。其中,CE_(0.95)LA_(0.05)O_单片催化剂具有最高的CH 3 OH转化率和DMC产率,其与XPS测量的氧空位含量好。最后,CE_(0.95)LA_(0.05)O_单片催化剂还显示出超过100小时的优异耐久性,主要是由于镧系含量掺入催化剂结构和表面性质的氧化铈中的掺杂效应。

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