Reaction
mechanisms and catalysis in the one-step synthesis of methylal via
methanol oxidation
Meng Yuana,c, Mengru Donga, Zhiwei
Tiane, Yuanjun Cheb, Yuanyu
Tiana,c,d*,
Yingyun Qiaoa,c*, Jinhong Zhang a,c,
Dawei Li a,c
aState
Key Laboratory of Heavy Oil
Processing,
China
University of Petroleum (East China), Qingdao Shandong
266580,
China.
b School of Environmental and Chemical Engineering,
Xi’an Polytechnic University, Xi’an, Shaanxi, 710048, China
c Shandong Engineering and Technology Research Center
of High Carbon Low Carbonization, China University of Petroleum (East
China), Qingdao 266580, PR China
d Key Laboratory
of Low Carbon Energy and Chemical Engineering,
Shandong
University of Science and Technology, Qingdao Shandong 266590, China.
e Jiangsu Co-Innovation Center of Efficient Processing
and Utilization of Forest Resources, International Innovation Center for
Forest Chemicals and Materials, College of Materials Science and
Engineering, Nanjing Forestry University, Nanjing, 210037, China.
*Corresponding author. Tel.: +86-0532-86057766. E-mail
addresses:
tianyy1008@126.com (Y.
Tian);
qiao_yingyun@126.com
(Y. Qiao)
Abstract :
This paper reports on the scaling-up of a one-step methanol production
process from the laboratory scale to the pilot scale. This lays the
foundation for the industrialization of a one-step process for preparing
DMM from methanol. After a long period of operation in the circulating
fluidized bed, the Fe-Mo/HZSM-5 catalyst was shown to have high
stability and carbon deposition resistance, and the regeneration effect
of the circulating regeneration fluidized bed was better. In addition,
in-situ DRIFTS was used to explore the effects of reaction time, the
Mo-Fe ratio and carrier Si-Al ratio on the reaction and product
distribution. It was found that the synergistic effect of oxidation
centers and acid centers was the fundamental reason for the excellent
catalytic performance of the Fe-Mo/HZSM-5 catalyst. And proposed the
reaction mechanisms in the one-step synthesis of methylal via methanol
oxidation.
Key words: DMM, Pilot-scale process, In-situ DRIFTS, Reaction
mechanisms