燃料化学学报2017，Vol.45Issue(9)：1114-1121,8.
不同前驱体制备的SO42-/AC催化剂在二甲醚直接氧化合成聚甲氧基二甲醚中的反应性能
Performance of SO42-/AC catalysts prepared with different precursors in the synthesis of polyoxymethylene dimethyl ethers from dimethyl ether direct oxidation
摘要
Abstract
A series of SO24-/AC bifunctional catalysts,in which SO42-and AC acted as the acid sites and redox sites,respectively,are prepared by impregnation with H2 SO4 and (NH4)2 SO4 as precursors and active carbon as support;their catalytic performance in the direct oxidation of dimethyl ether (DME) to polyoxymethylene dimethyl ethers (DMMx) was investigated.The results show that the catalytic performance of SO24-/AC catalysts is significantly related to the precursor used.Over the 40％ H2SO4/AC catalyst,the selectivity to DMM1-2 reaches 59.7％,with a DME conversion of 8.4％;in addition,there is no COx observed in the products.However,a large amount of COx by-product is formed over the 40％ (NH4) 2SO4/AC catalyst;meanwhile,the selectivity to DMM is only 2.7 ％ and no DMM2 is formed.The XRD,N2 sorption,NH3-TPD and O2-TPD-MS characterization results illustrate that the suitable amount of weak acid sites and redox sites of the H2SO4/AC catalyst is beneficial to the formation of long chain DMMx from DME oxidation.The modification of AC with SO42-promotes the activation of O2 over the surface of AC support,whereas the introduction of H2 SO4 improves the weak acid sites of the catalyst.On the contrary,the number of medium-strong acid sites of the catalyst is increased by modifying AC with (NH4)2SO4.关键词
二甲醚/聚甲氧基二甲醚/直接氧化/前驱体/SO42-/ACKey words
dimethyl ether/polyoxymethylene dimethyl ethers/direct oxidation/precursor/SO24-/AC分类
化学化工引用本文复制引用
高秀娟,王文峰,顾颖颖,张振洲,张清德,韩怡卓,谭猗生..不同前驱体制备的SO42-/AC催化剂在二甲醚直接氧化合成聚甲氧基二甲醚中的反应性能[J].燃料化学学报,2017,45(9):1114-1121,8.基金项目
This work was financially supported by the National Natural Science Foundation of China (21373253,20903114) and Youth Innovation Promotion Association CAS (2014155).国家自然科学基金(21373253,20903114)和中国科学院青年创新促进会(2014155)资助 （21373253,20903114）
