用氟化钾对 Ti-MWW 沸石进行丙烯环氧化后处理

IF 4.3 3区 工程技术 Q2 ENGINEERING, CHEMICAL Frontiers of Chemical Science and Engineering Pub Date : 2024-05-30 DOI:10.1007/s11705-024-2441-1
Xintong Li, Xianchen Gong, Jilong Wang, Shengbo Jin, Hao Xu, Peng Wu
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摘要

用过氧化氢(HPPO)将丙烯环氧化成环氧丙烷(PO)是一种环境友好且具有成本效益的工艺,其中钛硅酸盐可用作催化剂。Ti-MWW 是该工艺的一种潜在工业催化剂,该工艺涉及将 HPPO 加入到 PO 中。二次结晶过程中产生的硅烷醇基团不可避免地会导致 PO 的开环和 HPPO 的低效分解,从而降低了 PO 的选择性和 Ti-MWW 的使用寿命。为了解决这个问题,我们用氟化钾水溶液对结构化 Bf-Ti-MWW 催化剂进行了后处理改性。通过用氟化钾淬灭硅烷醇基团并在 Ti-MWW 框架中植入电子吸收氟化基团,催化活性和 HPPO 利用效率都得到了提高。此外,还禁止了 PO 的开环反应。在连续固定床液相丙烯环氧化反应中,经 KF 处理的结构化 Ti-MWW 催化剂的寿命长达 2700 h,PO 产率为 590 g-kg-1-h-1。
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Post-treatment of Ti-MWW zeolite with potassium fluoride for propylene epoxidation

Epoxidation of propylene to propylene oxide (PO) with hydrogen peroxide (HPPO) is an environmentally friendly and cost-efficient process in which titanosilicates are used as catalysts. Ti-MWW is a potential industrial catalyst for this process, which involves the addition of HPPO to PO. The silanol groups generated during secondary crystallization unavoidably result in ring-opening of PO and inefficient decomposition of HPPO, which diminish the PO selectivity and the lifespan of Ti-MWW. To address this issue, we conducted post-treatment modifications of the structured Bf-Ti-MWW catalyst with potassium fluoride aqueous solutions. By quenching the silanol groups with potassium fluoride and implanting electron-withdrawing fluoride groups into the Ti-MWW framework, both the catalytic activity and HPPO utilization efficiency were increased. Moreover, the ring opening reaction of PO was prohibited. In a continuous fixed-bed liquid-phase propylene epoxidation reaction, the KF-treated structured Ti-MWW catalyst displayed an exceptionally long lifespan of 2700 h, with a PO yield of 590 g·kg−1·h−1.

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来源期刊
CiteScore
7.60
自引率
6.70%
发文量
868
审稿时长
1 months
期刊介绍: Frontiers of Chemical Science and Engineering presents the latest developments in chemical science and engineering, emphasizing emerging and multidisciplinary fields and international trends in research and development. The journal promotes communication and exchange between scientists all over the world. The contents include original reviews, research papers and short communications. Coverage includes catalysis and reaction engineering, clean energy, functional material, nanotechnology and nanoscience, biomaterials and biotechnology, particle technology and multiphase processing, separation science and technology, sustainable technologies and green processing.
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