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...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.展开更多
基金the fund from the National Natural Science Foundation of China(22208349)the Innovation Academy for Green Manufacture(Chinese Academy of Sciences,IAGM2020C20)+1 种基金Shandong Provincial Natural Science Youth Fund(ZR2022QB244)Japan Society for the Promotion of Science(P20345)。
文摘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.
