碳酸二甲酯
甲醇
铈
催化作用
氧化铈
锆
氧化物
无机化学
金属
金属有机骨架
X射线光电子能谱
材料科学
化学
核化学
化学工程
有机化学
物理化学
吸附
冶金
工程类
作者
Linmeng Huo,Lin Wang,Jingjie Li,Yanfeng Pu,Keng Xuan,Congzhen Qiao,Hao Yang
标识
DOI:10.1016/j.jcou.2022.102352
摘要
The disadvantage of Ce/Zr metal oxide as catalyst for direct synthesis dimethyl carbonate (DMC) from CO2 and methanol is low DMC formation rate because of its low specific surface area and active sites. In this work, it can be improved by highly uniform dispersion cerium doped Zr-based metal-organic frameworks (UiO-66 MOFs), which were synthesized via a modified hydrothermal method. The as-prepared catalysts have been extensively characterized using XRD, BET, FT-IR, SEM, TEM, TGA, NH3-TPD, CO2-TPD, XPS techniques. Experimental evaluation results indicated that the highly uniform dispersed Ce-doped UiO-66 MOFs exhibited markedly improved catalytic performance than traditional Ce/Zr metal oxide catalyst. The highest yield of DMC catalyzed by Ce-UiO-66–2 was 0.295% (reaction time was 12 h; reaction temperature was 140 °C; reaction pressure was 11 MPa). Then, it was found that doping of Ce atoms into the zirconium lattice to produce UiO-66 MOFs could effectively increase the number of acidic and medium basic sites than UiO-66 (none Ce), thus could greatly enhance the catalytic performance. Moreover, using 2-cyanopyridine as dehydrating agent, the DMC yield could be further raised greatly. Last, based on reported literature and our results, a possible reaction mechanism over Ce-UiO-66-X was proposed.
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