用过氧化氢氧化醇的磷钨阴离子基咪唑多孔离子聚合物

IF 4.5 3区 材料科学 Q1 CHEMISTRY, APPLIED Microporous and Mesoporous Materials Pub Date : 2025-05-15 Epub Date: 2025-03-04 DOI:10.1016/j.micromeso.2025.113571
Lin Lei , Jiaxian Chen , Jinhong Xiao , Yongjian Qiu , Qinggang Ren , Yaju Chen , Hongbing Ji
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引用次数: 0

摘要

采用一锅Friedel-Crafts烷基化-季铵化反应和阴离子交换法制备了咪唑基超交联多孔离子聚合物(IHPiP)固定化磷钨(PW)阴离子杂化催化剂(IHPiP-PW)。所得的IHPiP-PW具有615 m2 g−1的高比表面积,含有丰富的分层孔隙。IHPiP-PW可有效地将1-苯乙醇与H2O2氧化成苯乙酮,转化率高达95.7%,并具有定量选择性。当底物/PW摩尔比为4000时,得到了3300个翻转次数和914.0 h−1的初始翻转频率。动力学研究表明,1-苯乙醇氧化符合准一级动力学,表观活化能为26.116 kJ mol−1。该催化体系耐多种底物。此外,IHPiP-PW可以很容易地回收并有效地重复使用6个循环,而没有明显的催化活性损失。
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Phosphotungstic anions-based imidazolium porous ionic polymer for oxidation of alcohols with hydrogen peroxide
An imidazolium-based hyper-crosslinked porous ionic polymer (IHPiP) immobilized phosphotungstic (PW) anions hybrid catalyst (IHPiP-PW) was synthesized based on a one-pot Friedel–Crafts alkylation and quaternization reaction, followed by anion exchange. The obtained IHPiP-PW exhibited a high specific surface area of 615 m2 g−1 containing plentiful hierarchical pores. IHPiP-PW was effective in the oxidation of 1-phenylethanol into acetophenone with H2O2 to give a high conversion of 95.7 % and quantitative selectivity. A remarkable turnover number of 3300 and initial turnover frequency of 914.0 h−1 were obtained at a substrate/PW molar ratio of 4000. Kinetic study demonstrated that 1-phenylethanol oxidation obeyed pseudo-first-order kinetics and the apparent activation energy was calculated to be 26.116 kJ mol−1. This catalytic system was tolerant of a wide range of substrates. Moreover, IHPiP-PW could be readily recovered and effectively reused for six cycles without significant catalytic activity loss.
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来源期刊
Microporous and Mesoporous Materials
Microporous and Mesoporous Materials 化学-材料科学:综合
CiteScore
10.70
自引率
5.80%
发文量
649
审稿时长
26 days
期刊介绍: Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.
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