Rhenium oxide-modified H3PW12O40/TiO2 catalysts for selective oxidation of dimethyl ether to dimethoxy dimethyl ether

被引:44
作者
Zhang, Qingde [1 ]
Tan, Yisheng [1 ]
Liu, Guangbo [1 ,2 ]
Zhang, Junfeng [1 ]
Han, Yizhuo [1 ]
机构
[1] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
基金
中国国家自然科学基金;
关键词
OLEFIN METATHESIS; LOW-TEMPERATURE; METHANOL; FORMALDEHYDE; METHYLAL; SUPPORT; ETHANOL; CH3REO3/NB2O5; GAMMA-AL2O3; PERFORMANCE;
D O I
10.1039/c4gc01373e
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
An efficient rhenium oxide-modified H3PW12O40/TiO2 catalyst is found for a new synthesis of dimethoxy dimethyl ether from dimethyl ether oxidation. The effects of Re loading, H3PW12O40 content and different feedstocks on the performance of Re-H3PW12O40/TiO2 were investigated. The results showed that DMM2 selectivity was significantly improved up to 60.0%, with 15.6% of DME conversion over 5% Re-20% H3PW12O40/TiO2. NH3-TPD, NH3-IR, Raman spectra, H-2-TPR, XPS and TEM were used to extensively characterize the structure and surface properties of the catalysts. The introduction of H3PW12O40 significantly affected the structure and reducibility of surface rhenium oxide species, in addition to increasing the acidity of the catalyst. The increased number of Lewis acid sites and weak acid sites and the optimal ratio of Re4+/Re7+ of Re-H3PW12O40/TiO2 were favorable for the formation of DMM2 from DME oxidation. The possible reaction pathway of DME oxidation to DMM2 was proposed.
引用
收藏
页码:4708 / 4715
页数:8
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