燃料化学学报（中英文）2026，Vol.54Issue(5)：125-137,13.DOI:10.1016/S1872-5813(26)60636-6
NASICON基催化材料上甲醇直接氧化制聚甲氧基二甲醚研究
Research on direct oxidation of methanol to polyoxymethylene dimethyl ethers over NASICON-based catalytic materials
摘要
Abstract
Polyoxymethylene dimethyl ethers(DMMx)are highly promising clean diesel additives.Compared to the traditional aldol condensation route,the one-step oxidative method for producing DMMx directly from methanol is a green synthesis route offering significant advantages.However,due to the complexity of the reaction,a balance must be struck between oxidation depth and C-O chain growth efficiency.This imposes specific requirements on the design of catalysts with multifunctional active sites:the catalyst should possess appropriate oxidative activity,suitable acid strength distribution,and effective synergy between these two functions.To address these challenges,this study designed a sulfuric acid-modified molybdenum-doped NASICON catalyst,which demonstrated favorable catalytic performance in the one-step oxidative synthesis of DMMx from methanol.Over the NSC-Mo-0.5-30％catalyst,methanol conversion rate of 81.3％and the DMMx selectivity of 58.7％were achieved,along with the formation of heavier molecules,as evidenced by the DMM2-6 selectivity of 11.3％.The NH3-TPD,Py-IR and XPS results indicate that the introduction of molybdenum increases the number of weak Lewis acid sites,while sulfuric acid impregnation not only generates gradient-distributed Brønsted acid sites but also promotes the formation of Mo5+/Mo6+redox pairs.The cooperation of the two types of active sites significantly enhances catalyst performance.关键词
甲醇/NASICON材料/聚甲氧基二甲醚/C-O链增长/氧化Key words
methanol/NASICON material/polyoxymethylene dimethyl ethers/C-O chain growth/oxidation分类
化学化工引用本文复制引用
程义涛,王夏青,高秀娟,宋法恩,王晓星,武应全,张俊峰,韩怡卓,张清德..NASICON基催化材料上甲醇直接氧化制聚甲氧基二甲醚研究[J].燃料化学学报（中英文）,2026,54(5):125-137,13.基金项目
Supported by the National Natural Science Foundation of China(22172187),the Autonomous Research Project of SKLCC(2024BWZ012),the Innovation Foundation of ICC-CAS(SCJC-DT-2023-05)and the Youth Innovation Promotion Association CAS(2014155). （22172187）
