Effects of the support on bifunctional one-step synthesis of methylal via methanol oxidation catalysed by Fe-Mo-based bifunctional catalysts

被引:12
|
作者
Yuan, Meng [1 ,4 ]
Tang, Ruiyuan [2 ]
Sun, Xiangyu [3 ]
Zhang, Zhimei [1 ,4 ]
Tian, Yuanyu [1 ,4 ,5 ]
Qiao, Yingyun [1 ,4 ]
机构
[1] China Univ Petr East China, State Key Lab Heavy Oil Proc, Qingdao 266580, Shandong, Peoples R China
[2] Xian Shiyou Univ, Res Ctr Petr Proc & Petrochem, Xian 710065, Shanxi, Peoples R China
[3] China Univ Petr East China, Coll Petr Engn, Qingdao 266580, Peoples R China
[4] China Univ Petr East China, Shandong Engn & Technol Res Ctr High Carbon Low C, Qingdao 266580, Peoples R China
[5] Shandong Univ Sci & Technol, Key Lab Low Carbon Energy & Chem Engn, Qingdao 266590, Shandong, Peoples R China
基金
中国国家自然科学基金;
关键词
POLYOXYMETHYLENE DIMETHYL ETHERS; ACIDIC IONIC LIQUIDS; SELECTIVE OXIDATION; EFFICIENT CATALYSTS; CO METHANATION; DIMETHOXYMETHANE; PERFORMANCE; ZEOLITES; OXIDE; TRANSFORMATION;
D O I
10.1039/d0se01194k
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
In the one-step preparation of methylal from methanol, achieving high methanol conversion and high methylal yield is a huge challenge. To address this problem, in this study a new Fe-Mo-based catalyst was designed, and the effect of the type and amount of the support on catalytic activity was explored. The results showed that Mo:Fe(2)/HZSM-5(80 + 80), in which HZSM-5(80 + 80) was the catalytic support, had excellent catalytic performance, with the yield of methylal reaching 81.33%, much higher than other reported results of this process. Through XPS, NH3-TPD and PY-FTIR analyses it was found that the formation of Mo5+ promoted coordination of the two terminal oxygens with the Mo double bond in the Fe-2(MoO4)(3) octahedron, and the higher the B/L acid site ratio, the better the catalytic activity and the higher the selectivity of the target product. The apparent activation energy also further proved that Mo:Fe(2)/HZSM-5(80 + 80) was highly suitable for the one-step production of methylal from methanol.
引用
收藏
页码:246 / 260
页数:15
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