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

来源：

JOURNAL OF CATALYSIS | 2025年 / 443卷

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.

引用

页数：10