Abstract
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 (Ce1-xLaxOδ nanocomposites, x=0.00, 0.05, 0.10, 0.15, and 0.20) via a co-precipitation method. These Ce1-xLaxOδ composites are ground into slurry by ball milled and then coated on cordierite honeycomb ceramics to obtain Ce1-xLaxOδ monolithic catalysts. These Ce1-xLaxOδ composites are characterized extensively by TEM, XRD, Raman spectroscopy, N2 adsorption-desorption isotherms, H2-TPR and XPS. The characterization results show that the Ce1-xLaxOδ composites nanoparticles possesses richer surface oxygen vacancies, higher BET surface area and smaller particle size than that of pure CeO2 nanoparticle. Besides, catalytic activity test shows these Ce1-xLaxOδ monolithic catalysts exhibit better catalytic performance than that of pure CeO2 nanoparticles. Among them, Ce0.95La0.05Oδ 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 Ce0.95La0.05Oδ 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.
Highlights
With the development of industry and extensive use of petrochemical resources, the increased greenhouse gas emissions have caused shocking climate change, which causes huge environmental problems [1], such as global warming
Based on the wide application and large demand of Dimethyl carbonate (DMC), researchers recently have discovered a series of methods for the DMC synthesis, including carbonylation of methanol [9, 10], transesterification of carbonates [11, 12], alcoholysis of urea [13] and direct synthesis from CO2 and methanol [14,15,16,17]
After the reaction system was heated to the required temperature, a constant current pump was used to introduce CH3OH into the system to participate in the reaction
Summary
With the development of industry and extensive use of petrochemical resources, the increased greenhouse gas emissions have caused shocking climate change, which causes huge environmental problems [1], such as global warming. Based on the wide application and large demand of DMC, researchers recently have discovered a series of methods for the DMC synthesis, including carbonylation of methanol [9, 10], transesterification of carbonates [11, 12], alcoholysis of urea [13] and direct synthesis from CO2 and methanol [14,15,16,17] Among all of these routes, CO2 + 2CH3OH → CH3OC(=O)OCH3 + H2O, this synthesis method has gradually become the most attractive method, which can realize the efficient use of the greenhouse gas CO2 [17]. The experimental results show that the lanthanum doped ceria monolithic catalysts exhibit excellent catalytic activity and great stability in DMC direct synthetic method in the absence of any dehydrating agents
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