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