Studies on polyoxymethylene dimethyl ethers production from dimethoxymethane and 1,3,5-trioxane over SO_(4)^(2-)/ZrO_(2)-TiO_(2)  

作　　者：Haoyu Yao Jiangcheng Li Jiangyan Li Xiangfeng Liang Gang Wang Haiyan Luo 

机构地区：[1]Environmental Resources,Green Chemical Separation Group,Qingdao Institute of Bioenergy,Bioprocess Technology,Chinese Academy of Sciences,Qingdao 266101,China [2]Beijing Insight Chemistry Co.,Ltd,Beijing 101121,China [3]Merck Sharp&Dohme Research and Development(China)Co.,Ltd,Beijing 100101,China [4]Institute for Catalysis,Hokkaido University,N-21,W-10,Sapporo 001-0021,Japan [5]CAS Key Laboratory of Green Process and Engineering,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190,China

出　　处：《Chinese Journal of Chemical Engineering》2023年第9期24-36,共13页中国化学工程学报（英文版）

基　　金：the fund from the National Natural Science Foundation of China(22208349);the Innovation Academy for Green Manufacture(Chinese Academy of Sciences,IAGM2020C20);Shandong Provincial Natural Science Youth Fund(ZR2022QB244);Japan Society for the Promotion of Science(P20345)。

摘　　要：Polyoxymethylene dimethyl ethers(OMEs)with physical properties similar to those of diesel has received significant attention as green additives for soot emission suppression.Herein,series of SO_(4)^(2-)/ZrO_(2)-TiO_(2)catalysts were developed for OMEs production from dimethoxymethane(DMM)and1,3,5-trioxane through sequential formaldehyde monomer insertion into C-O bond of DMM.Not Lewis but Bronsted acid sites were identified to be active for the decomposition of 1,3,5-trioxane into formaldehyde unit,however,both of them are effective for the chain propagation of DMM via formaldehyde unit insertion into C-O bond.Kinetic studies indicated each chain growth step exhibited the same parameters and activation barrier on corresponding Bronsted and Lewis acid sites due to the same reaction mechanism and very similar chemical structure of OMEs.Also,the catalytic stability investigation suggested the deactivation behavior was derived from the carbon deposition,and the decay factor could be exponentially correlated with the amount of coke accumulation.

关 键 词：Polyoxymethylene dimethylethers SO_(4)^(2-)/ZrO_(2)-TiO_(2) Chain propagation Kinetics Deactivation behavior 

分 类 号：O64[理学—物理化学]