The Synergistic Action of Co, Cu and Ce Was Used to Achieve Efficient Aerobic Epoxidation of Styrene

IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL
Tong Li, Fuliang Liu, Xiaofang Wang, Zhaohao Han, Xiaoqiong Jia, Ping Wang, Qingyan Chu, Yuxuan Sheng
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Abstract

The precise embedding of metal species within specific sites of zeolite frameworks and their unique microenvironments exert fascinating influences on catalytic performance. Herein, we report the rational design of a highly efficient Co-Cu@CTS-1 catalyst through the strategic incorporation of Co, Cu, and Ce into TS-1 zeolite, where Ce is doped at silicon atomic sites while Co and Cu are encapsulated within the zeolite cages. Mechanistic investigations reveal that the synergistic interplay among Co, Cu, and Ce is pivotal for catalytic activity: Co facilitates molecular oxygen activation to generate reactive oxygen species (O⁻), while Ce(III) enhances oxygen vacancy concentration, significantly boosting styrene conversion. Moreover, the distinctive electronic interaction between Ce and Cu markedly improves the selectivity toward styrene oxide. The optimized Co-Cu@CTS-1 catalyst exhibits exceptional performance in the aerobic epoxidation of styrene, achieving a remarkable conversion of 78.11% with 87.31% epoxide selectivity under mild conditions (80 °C, 2 h). Furthermore, the catalyst demonstrates outstanding stability, retaining 68.21% conversion even after 20 reaction cycles, underscoring its superior resistance to metal sintering and long-term durability. This work provides valuable insights into the rational design of multifunctional zeolite catalysts through precise metal positioning and microenvironment modulation.

Graphical Abstract

Abstract Image

利用Co、Cu和Ce的协同作用实现苯乙烯的高效好氧环氧化反应
金属物种在沸石框架的特定位点内的精确嵌入及其独特的微环境对催化性能产生了迷人的影响。本文中,我们通过将Co, Cu和Ce战略性地掺入TS-1沸石中,合理设计了一种高效的Co-Cu@CTS-1催化剂,其中Ce掺杂在硅原子位置,而Co和Cu被封装在沸石笼中。机理研究表明,Co, Cu和Ce之间的协同作用是催化活性的关键:Co促进分子氧活化产生活性氧(O -毒血症),而Ce(III)提高氧空位浓度,显著促进苯乙烯转化。此外,Ce和Cu之间独特的电子相互作用显著提高了对苯乙烯氧化物的选择性。优化后的Co-Cu@CTS-1催化剂在苯乙烯的好氧环氧化反应中表现出优异的性能,在温和的条件下(80℃,2 h),环氧化转化率为78.11%,环氧化物选择性为87.31%。此外,该催化剂表现出出色的稳定性,即使在20个反应循环后仍保持68.21%的转化率,突出了其优越的抗金属烧结性能和长期耐久性。这项工作为通过精确的金属定位和微环境调节来合理设计多功能沸石催化剂提供了有价值的见解。图形抽象
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来源期刊
Catalysis Letters
Catalysis Letters 化学-物理化学
CiteScore
5.70
自引率
3.60%
发文量
327
审稿时长
1 months
期刊介绍: Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.
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