Efficient cerium oxide catalysts for the direct synthesis of dimethyl carbonate from carbon dioxide: characterization, catalytic activity, and thermodynamic studies

IF 3.5 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY
Jingjing Peng, Xiaoling Xu, Yiying Zhang, Yu Chen, Yansheng Liu
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Abstract

Using oxygen vacancies to modify the surface properties of catalysts to enhance catalytic activity, inhibiting reverse reactions can effectively increase synthetic yield. This study presents an M-CeO2 catalyst derived from MOF-808(Ce), which was successfully applied to the synthesis of dimethyl carbonate (DMC) under dehydration agent-free conditions. Particularly, it has been found that M-CeO2 catalyst enables the formation of defective microporous structure in ceria catalysts, enriching the surfaces with oxygen vacancy sites, and slowing down the reverse reaction. This leads to the yield of DMC reaching 4.184 mmol/g, corresponding to a significant improvement in the conversion rate of methanol up to 1.42%. Moreover, the M-CeO2 catalyst exhibited over 1.6 times higher methanol conversion rate than reflux-synthesized ceria nanorods, which can be attributed to their superior CO2 adsorption and activation capability, as well as the inhibition of reverse reactions. These conclusions are supported by combined surface characterizations and thermodynamic calculations. We developed a novel method for surface engineering of catalysts whose function was combined with dehydrating agents. A possible reaction mechanism for the synthesis of DMC from CO2 and CH3OH on M-CeO2 was proposed.

二氧化碳直接合成碳酸二甲酯的高效氧化铈催化剂:表征、催化活性和热力学研究
利用氧空位修饰催化剂的表面性质,提高催化活性,抑制逆反应,可有效提高合成收率。以MOF-808(Ce)为原料制备了M-CeO2催化剂,并成功应用于无脱水条件下合成碳酸二甲酯(DMC)。特别是,研究发现M-CeO2催化剂能使铈催化剂形成缺陷微孔结构,使其表面富氧空位,减缓逆反应。这使得DMC的产率达到4.184 mmol/g,相应的甲醇转化率提高了1.42%。此外,M-CeO2催化剂的甲醇转化率比回流合成的二氧化铈纳米棒高1.6倍以上,这可归因于其优越的CO2吸附和活化能力,以及对逆反应的抑制作用。这些结论得到了表面表征和热力学计算的支持。提出了一种结合脱水剂作用的催化剂表面工程新方法。提出了CO2和CH3OH在M-CeO2上合成DMC的可能反应机理。
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来源期刊
Journal of Materials Science
Journal of Materials Science 工程技术-材料科学:综合
CiteScore
7.90
自引率
4.40%
发文量
1297
审稿时长
2.4 months
期刊介绍: The Journal of Materials Science publishes reviews, full-length papers, and short Communications recording original research results on, or techniques for studying the relationship between structure, properties, and uses of materials. The subjects are seen from international and interdisciplinary perspectives covering areas including metals, ceramics, glasses, polymers, electrical materials, composite materials, fibers, nanostructured materials, nanocomposites, and biological and biomedical materials. The Journal of Materials Science is now firmly established as the leading source of primary communication for scientists investigating the structure and properties of all engineering materials.
文献相关原料
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麦克林
Ce(NO3)3?6H2O
麦克林
Anhydrous ethanol
麦克林
Anhydrous methanol
阿拉丁
Trimesic acid
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