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- Title
Rational construction of multiple hollow silicalite-1 zeolite with enhanced quasi acidity for robust vapor-phase Beckmann rearrangement.
- Authors
Zhang, Peng; Yi, Xianfeng; Xia, Changjiu; Peng, Xinxin; Zhang, Shuai; Li, Chengxiang; Zheng, Anmin; Zhang, Xiaoxin; Luo, Yibin; Cui, Lifeng; Yu, Fuhong; Shu, Xingtian
- Abstract
Developing efficient and stable zeolites for vapor-phase Beckmann rearrangement of cyclohexanone oxime is still a great challenge to realize ε-caprolactam (CPL) green production. In this work, the hierarchical porous silicalite-1 zeolites with multiple hollow structure (S-1-M) are explored by in-situ desilication—recrystallization post-treatment of spongy highway-like zeolites (S-1-S), which are synthesized through silanization synthesis of conventional bulky silicalite-1 (S-1). Compared to S-1, S-1-M achieves superior catalytic performance, with improving the CPL selectivity from 85.7% to 94.1% and prolonging the catalyst lifetime from 74 to 126 h at a weight hourly space velocity (WHSV) of 6 h−1. Comprehensive physiochemical studies demonstrate that the highly dispersed intracrystalline cavities within S-1-M endow greater mass diffusion and better quasi acidity inducing by the enhanced H-bonds among abundant H-bonded silanols, which is cooperatively responsible for its superior catalytic performance.
- Subjects
BECKMANN rearrangement; ACIDITY; RECRYSTALLIZATION (Metallurgy); SILANOLS; ZEOLITES; SILANIZATION; CLAISEN rearrangement
- Publication
Nano Research, 2023, Vol 16, Issue 5, p7958
- ISSN
1998-0124
- Publication type
Article
- DOI
10.1007/s12274-022-5305-3