文献类型：期刊文献

英文题名：Modulating the Mn-O strength of OMS-2 by alkali metal doping for the catalytic oxidation of N, N-dimethylformamide

作者：Ye, Dongsheng[1];Cheng, Liang[1];Gao, Yanzhao[1];Li, Mingqi[1];Zhan, Wangcheng[1];Wang, Li[1];Guo, Yun[1];Dai, Qiguang[1];Wang, Aiyong[1];Guo, Yanglong[1]

机构：[1]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, State key Lab green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China

年份：2024

卷号：351

外文期刊名：SEPARATION AND PURIFICATION TECHNOLOGY

收录：;EI(收录号：20242216155828);WOS:【SCI-EXPANDED(收录号:WOS:001246209800001)】；

基金：This work was supported by the National Key Research and Devel- opment Program of China (2023YFA1508500, 2022YFB3504200, 2023YFC3707500) , the National Natural Science Foundation of China (22106101, U21A20326) and the Fundamental Research Funds for the Central Universities.

语种：英文

外文关键词：DMF oxidation; OMS-2; Alkali metal doping; Oxygen mobility

摘要：Promoting catalytic activity by engineering oxygen mobility and reactivity is an intriguing approach to heterogeneous catalysis. Through the cation -exchange method, alkali metals were introduced into the OMS-2 catalyst, resulting in a weakening of internal Mn-O bonds and an increase in surface oxygen vacancies. Alkali metal doping significantly enhanced the catalytic activity of OMS-2 in the catalytic oxidation of N, N-dimethylformamide (DMF). Specifically, Rb-OMS-2, obtained by doping of Rb into OMS-2, displayed the highest oxygen vacancy, oxygen mobility and reactive lattice oxygen. The Rb-OMS-2 catalyst displayed better catalytic performance with 100 % CO 2 yield, lowest N 2 O concentration and excellent water resistance, and stabilized at 220 degrees C for more than 120 h. In situ DRIFTS revealed that DMF molecules reacted with three kinds of oxygen species, then breakage of the C-N bond occurred, finally the remaining C -containing groups were subsequently oxidized to CO 2 , and intermediates of -NH 2 and -NO + reacted to form N 2 .