用于 1-己烯加氢甲酰化的高效中空 Rh@H-S-1 催化剂

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-09-21 DOI:10.1016/j.jcat.2024.115770
Gongcheng Sun, Subing Fan, Junmin Lv, Tiansheng Zhao
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引用次数: 0

摘要

采用有机碱处理和重结晶的方法制备了具有 "蛋壳 "结构的中空沸石包覆 Rh 催化剂 Rh@H-S-1。与直接封装的 Rh@S-1 催化剂和表面浸渍的 Rh/S-1 催化剂相比,由于 Rh 的高分散性和高扩散性,该催化剂在 1- 己烯的加氢甲酰化反应中表现出更高的活性和更高的 TOF 值。在制备过程中,Rh 元素无需还原,可在合成气中就地还原。随着反应过程的进行,低价态 Rhδ+ 的含量逐渐增加,并成为活性中心。在 CO 和 H2 的协同作用下,低氧化态的 Rh+ 或 Rh(CO)2 形式的 Rhδ+ 被认为是加氢甲酰化过程中的活性位点。重要的是,与浸渍的 Rh/S-1 催化剂相比,中空封装催化剂能有效地将 Rh 浸出降至 0.1 ppm,并表现出更好的稳定性。
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Effective hollow Rh@H-S-1 catalyst for hydroformylation of 1-hexene
A hollow zeolite encapsulated Rh catalyst Rh@H-S-1 with an “eggshell” structure was prepared using the method of organic alkali treatment and recrystallization. Compared with catalysts with directly encapsulated Rh@S-1 and surface impregnated Rh/S-1, this catalyst exhibited both superior activity and a higher TOF value in hydroformylation of 1-hexene due to the high dispersion of Rh and high diffusion. The Rh element did not need to be reduced in the preparation, and it was in situ reduced by the syngas. The content of lower valence Rhδ+ gradually increased with the reaction procedure and played as an active center. The low oxidized state Rh+ or Rhδ+ in the form of Rh(CO)2 are proposed as active sites in hydroformylation, which were generated under the synergistic effect between CO and H2. Importantly, the hollow encapsulated catalyst effectively decreased Rh leaching to 0.1 ppm and showed better stability compared with the impregnated Rh/S-1 catalyst.
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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