Enhanced catalytic performance of NH4+-exchanged Ti-MWW zeotypes for the liquid-phase epoxidation of alkenes with H2O2

被引:0
作者
Wang, Yuexia [1 ]
Xu, Jiaqi [1 ]
Lin, Xuan [1 ]
Liu, Chaosi [1 ]
Lu, Xinqing [1 ,2 ]
Gao, Yijing [1 ,2 ]
Pepe, Francesco [3 ]
Caputo, Domenico [4 ]
Zhu, Weidong [1 ,2 ]
机构
[1] Zhejiang Normal Univ, Inst Adv Fluorine Containing Mat, Zhejiang Engn Lab Green Synth & Applicat Fluorine, Jinhua 321004, Peoples R China
[2] Zhejiang Normal Univ, Inst Phys Chem, Key Lab Minist Educ Adv Catalysis Mat, Jinhua 321004, Peoples R China
[3] Univ Sannio, Dept Engn, Piazza Roma 21, I-82100 Benevento, Italy
[4] Univ Naples Federico II, Dept Chem Mat & Prod Engn, ACLabs Appl Chem Labs, Ple V Tecchio 80, I-80125 Naples, Italy
关键词
Ti-MWW zeotype; Density Functional Theory; -Ti-OOH hydroperoxo intermediates; Alkene epoxidation; OXIDATIVE HYDRATION; SELECTIVE SYNTHESIS; HYDROGEN-PEROXIDE; TS-1; ZEOLITE; TITANOSILICATE; ETHYLENE; OXIDE; CONSTRUCTION; EFFICIENCY; POINTS;
D O I
10.1016/j.jcat.2025.115982
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Ti-MWW zeotypes, characterized by their unique dual pore architecture consisting of intralayer 10-membered ring (MR) pore channels and additional interlayer 10-MR pore channels that are interconnected to intracrystalline 12-MR supercages, exhibit a remarkably catalytic superiority in the selective oxidation of small and/ or linear alkenes with hydrogen peroxide (H2O2), surpassing other titanosilicate zeotypes in performance. However, a further improvement on their catalytic performance is still needed for the industrialization of alkene epoxidation over Ti-MWW. In the present work, the introduction of NH4+ species into Ti-MWW was conducted via a facile but effective treatment of the as-synthesized zeotypes with NH4Cl, named N-Ti-MWW. The comprehensive characterization of N-Ti-MWW, derived from NH4+-exchanged Ti-MWW, coupled with Density Functional Theory (DFT) calculations, conclusively demonstrates that the integration of NH4+ into Ti-MWW promotes the generation of -Ti-OOH hydroperoxo intermediates, resulting in a higher catalytic activity in alkene epoxidation in comparison to the parent one. Moreover, the solvolysis of epoxides is significantly suppressed on N-Ti-MWW, enabling the catalyst to display a superior selectivity towards the targeted epoxide, thereby improving its overall catalytic performance. Additionally, N-Ti-MWW is reusable, after the regeneration of the deactivated catalyst simply treated with NH4Cl. As a result, it is anticipated that N-Ti-MWW would be applicable in the industrial epoxidation of alkenes with H2O2.
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页数:10
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