多孔聚噻吩聚合物负载Cu-Cu2O纳米颗粒高效催化醇氧化 |
Efficient aerobic oxidation of alcohols over Cu-Cu2O nanoparticles supported on a porous polythiophene polymer |
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摘要: 通过噻吩的氧化偶联反应,制得富含N、S杂原子的多孔有机聚合物PTPA。然后利用溶剂热法,合成了PTPA负载Cu-Cu2O的复合材料Cu-Cu2O/PTPA,并通过红外光谱(IR)、X射线衍射(XRD)、热重分析(TGA)、N2吸附-脱附、X射线光电子能谱(XPS)、扫描电镜(SEM)和高分辨透射电镜(HRTEM)等对其进行了全面表征。在30℃空气中的温和条件下,以2,2,6,6-四甲基哌啶氧化物(TEMPO)为助催化剂和N-甲基咪唑(NMI)为辅助配体,Cu-Cu2O/PTPA对苄醇、烯丙醇及杂环醇表现出良好的选择性催化氧化性能。这归因于该材料富含N、S杂原子,Cu-Cu2O/PTPA在催化苯甲醇氧化方面表现出优异的循环稳定性,重复使用9次后仍保持97%以上的产率。 |
关键词: 铜基催化剂 多孔有机聚合物 醇的选择性氧化 循环稳定性 |
基金项目: 浙江省自然科学基金一般项目(No.LY18B010007)资助。 |
Abstract: Porous organic polymer PTPA containing N, S heteroatoms has been prepared via oxidative coupling of thiophene. Then composite material Cu-Cu2O/PTPA was synthesized via solvothermal method and fully characterized by infrared spectroscopy (IR), X-ray diffraction (XRD), thermogravimetric analysis (TGA), N2 adsorption desorption, X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and high-resolution transmission electron microscopy (HRTEM). Under the mild conditions of 30 ℃ and open air, Cu-Cu2O/PTPA showed good catalytic activity towards selective oxidation of benzyl, allyl, and heterocyclic alcohols employing 2,2,6,6-tetrameth- ylpiperidine 1-oxyl (TEMPO) as a co-catalyst and N-methylimidazole (NMI) as an auxiliary ligand. Due to the high content of N and S heteroatoms in the material, Cu-Cu2O/PTPA showed excellent cycling stability for oxidation of benzyl alcohol, and the yield of product remained above 97% after 9 runs. |
Keywords: Cu-based catalyst porous organic polymers selective oxidation of alcohols cycling stability |
投稿时间:2023-03-09 修订日期:2023-05-19 |
摘要点击次数: 1943 |
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成佩颖,朱立华,吕春欣,刘江华,钟伟,何亚兵.多孔聚噻吩聚合物负载Cu-Cu2O纳米颗粒高效催化醇氧化[J].无机化学学报,2023,39(7):1223-1234. |
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