Polyoxymethylene dimethyl ethers synthesis from methanol and formaldehyde solution over one-pot synthesized spherical mesoporous sulfated zirconia  

作　　者：Xiangjun Li Shujun Li Xiaoping Wang Muhammad Asif Nawaz Dianhua Liu 

机构地区：[1]State Key Lab of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China

出　　处：《Chinese Journal of Chemical Engineering》2022年第6期161-172,共12页中国化学工程学报（英文版）

基　　金：This work was financially supported by National Key Research and Development Program of China(No.2018YFB0604804).

摘　　要：The synthesis of polyoxymethylene dimethyl ethers as an ideal diesel fuel additive is the current hot topic of modern petrochemical industry for their expedient properties in mitigating air pollutants emission during combustion.In this work,a series of spherical sulfated zirconia catalysts were prepared by a one-pot hydrothermal method assisted with surfactant cetyltrimethylammonium bromide(CTAB).The prepared sulfated zirconia catalysts were used to catalyze PODEn synthesis from methanol and formaldehyde solution.Various characterization(XRD,BET,SEM,TGA,NH_(3)-TPD,FTIR,and Py-IR)were employed to elaborate the structure–activity relationship of the studied catalytic system.The results demonstrated that S/Zr molar ratio in precursor solution played an effective role on catalyst morphology and acidic properties,where the weak Brønsted acid sites and strong Lewis acid sites were favorable to the conversion of methanol and formation of long-chain PODEn,respectively.The reaction parameters such as catalyst amount,molar ratio of FA/MeOH,reaction time,temperature and pressure were optimized.The speculated reaction pathway for PODEn synthesis was proposed based on the synergy of Brønsted and Lewis acid sites,which suggested that Brønsted and Lewis acid sites might be advantageous to the activation of polyoxymethylene hemiformals[CH_(3)(OCH_(2))_(n)OH]and methylene glycol(HOCH_(2)OH),respectively.

关 键 词：Polyoxymethylene dimethyl ethers Spherical sulfated zirconia METHANOL FORMALDEHYDE Reaction pathway Synergistic effect 

分 类 号：TE624.81[石油与天然气工程—油气加工工程]