Environment-friendly heterogeneous poly(ionic liquid)s immobilized polyoxometalate catalysts towards the efficient oxidation of alkenes

IF 3.9 2区化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2024-09-25 DOI:10.1016/j.mcat.2024.114572

Qiao Liu , Meirong Kang , Weiguo Fang , Hailong Liu , Zhiwei Huang

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Abstract

A novel quaternization reagent of (1E,1′E)-1,1′-(1,4-phenylene)bis(N-(3-(1H-imidazol-1-yl)propyl)methanimine) (PP) was synthesized and used for the preparation of a series of poly(ionic liquid)s (PILs) via the quaternization reaction. These PILs were subsequently loaded with polyoxometalates (POMs) to create innovative catalysts for the oxidation of alkenes. Comprehensive structural analysis of the catalysts showed that these PILs exhibited a high loading amount ratio of up to 542 % for POMs, which were well-dispersed on the surface of PILs. The PILs loaded POMs catalysts, especially for PW-PIL-TB-2PP with H₃PW₁₂O₄₀ as the POMs, displayed remarkable activity and stability in oxidizing cyclooctene, achieving a conversion rate of 97 % and a selectivity of 99 % for 1,2-epoxycyclooctane over six consecutive runs without notable loss. Furthermore, the PW-PIL-TB-2PP catalyst could also be used for the oxidation of a wide range of cyclic, linear, and aromatic alkenes.

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高效氧化烯烃的环境友好型多相固定聚（离子液体）聚氧化金属催化剂

我们合成了一种新型季铵化试剂 (1E,1′E)-1,1′-(1,4-亚苯基)双(N-(3-(1H-咪唑-1-基)丙基)甲亚胺) (PP)，并通过季铵化反应将其用于制备一系列聚离子液体 (PIL)。随后，这些聚离子液体负载了聚氧化金属盐（POMs），形成了用于氧化烯烃的创新催化剂。催化剂的全面结构分析表明，这些 PILs 的 POMs 负载率高达 542%，POMs 在 PILs 表面分散良好。负载 PILs 的 POMs 催化剂，尤其是以 H3PW12O40 为 POMs 的 PW-PIL-TB-2PP 催化剂，在氧化环辛烯时表现出显著的活性和稳定性，在连续六次运行中，1,2-环氧环辛烷的转化率达到 97%，选择性达到 99%，且无明显损失。此外，PW-PIL-TB-2PP 催化剂还可用于氧化多种环状、线性和芳香族烯烃。

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来源期刊

Molecular Catalysis Chemical Engineering-Process Chemistry and Technology

CiteScore

6.90

自引率

10.90%

发文量

700

审稿时长

40 days

期刊介绍： Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods