UiO-67-Sal-CuCl2在空气中催化芳香醇的选择性氧化

doi:10.7503/cjcu20180767

摘要/Abstract

摘要：

利用水热法一步合成了金属有机骨架(MOFs)材料UiO-67-Sal, 并将3种铜盐固定在其表面, 研究了3种铜MOFs材料催化芳香醇选择性氧化的性能. 结果表明, UiO-67-Sal-CuCl₂催化剂对芳香醇选择性氧化反应具有良好的催化活性, 且在重复使用4次后, 依然保持较好的催化效果.

关键词: 金属有机骨架材料, UiO-67, 芳香醇, 氧化, 选择性

Abstract:

Metal-organic-frameworks(MOFs) are a class of hybrid materials with unique porous structure. MOFs possess open pores of a permanent crystalline matrix, made of organic ligands and metal ions or clusters via coordination interactions. Permanently microporous MOFs materials have attracted considerable attention due to the large internal surface areas, uniform channels, thermal stability and other potential applications, such as gas separation and storage, catalysis, drug release and chemical sensing. The Zr-based MOF material(UiO-67-Sal) was functionalized through one-step hydrothermal synthesis, and the three copper(Ⅱ) salts were immobilized onto the UiO-67-salen. The three resulting Cu(Ⅱ)-UiO-67-Sal MOFs were evaluated for aerobic selective oxidation of a range of primary aromatic alcohols. The UiO-66-Sal-CuCl₂ catalyst exhibited excellent activity toward the selective erobic oxidation of primary aromatic alcohols using oxygen molecular as the oxygen source. Furthermore, the UiO-66-Sal-CuCl₂ catalyst showed a good recycle performance.

Key words: Metal-organic framework, UiO-67, Aromatic alcohol, Oxidation, Selectivity

中图分类号:

O625
O614

TrendMD:

钱文浩, 黄玮, 丛玉凤, 李富盛. UiO-67-Sal-CuCl₂在空气中催化芳香醇的选择性氧化. 高等学校化学学报, 2019, 40(6): 1178.

QIAN Wenhao,HUANG Wei,CONG Yufeng,LI Fusheng. Selective Oxidation of Benzyl Alcohols Catalyzed by UiO-67-Sal-CuCl₂ in Air^†. Chem. J. Chinese Universities, 2019, 40(6): 1178.

图/表 8

参考文献 33

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No.	Catalyst	Solvent	Base	Conversion^b(%)	Selectivity^b(%)
1	—	CH₃CN	NaHCO₃	0	—
2	CuCl₂	CH₃CN	NaHCO₃	81	99
3	Cu(NO₃)₂	CH₃CN	NaHCO₃	72	99
4	Cu(OAc)₂	CH₃CN	NaHCO₃	53	99
5	UiO-67-Sal	CH₃CN	NaHCO₃	0	—
6	UiO-67-Sal-Cu(NO₃)₂	CH₃CN	NaHCO₃	83	99
7	UiO-67-Sal-Cu(OAc)₂	CH₃CN	NaHCO₃	68	99
8	UiO-67-Sal-CuCl₂	CH₃CN	NaHCO₃	99	99
9	UiO-67-Sal-CuCl₂	1,4-Dioxane	NaHCO₃	82	99
10	UiO-67-Sal-CuCl₂	THF	NaHCO₃	78	99
11	UiO-67-Sal-CuCl₂	DMF	NaHCO₃	<5	99
12	UiO-67-Sal-CuCl₂	CH₃CN	NaOH	41	99
13	UiO-67-Sal-CuCl₂	CH₃CN	TEA	9	99

No.	Catalyst	Solvent	Base	Conversion^b(%)	Selectivity^b(%)
1	—	CH₃CN	NaHCO₃	0	—
2	CuCl₂	CH₃CN	NaHCO₃	81	99
3	Cu(NO₃)₂	CH₃CN	NaHCO₃	72	99
4	Cu(OAc)₂	CH₃CN	NaHCO₃	53	99
5	UiO-67-Sal	CH₃CN	NaHCO₃	0	—
6	UiO-67-Sal-Cu(NO₃)₂	CH₃CN	NaHCO₃	83	99
7	UiO-67-Sal-Cu(OAc)₂	CH₃CN	NaHCO₃	68	99
8	UiO-67-Sal-CuCl₂	CH₃CN	NaHCO₃	99	99
9	UiO-67-Sal-CuCl₂	1,4-Dioxane	NaHCO₃	82	99
10	UiO-67-Sal-CuCl₂	THF	NaHCO₃	78	99
11	UiO-67-Sal-CuCl₂	DMF	NaHCO₃	<5	99
12	UiO-67-Sal-CuCl₂	CH₃CN	NaOH	41	99
13	UiO-67-Sal-CuCl₂	CH₃CN	TEA	9	99

UiO-67-Sal-CuCl₂在空气中催化芳香醇的选择性氧化

Selective Oxidation of Benzyl Alcohols Catalyzed by UiO-67-Sal-CuCl₂ in Air^†

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No.	R	R'	Conversion^b(%)	Selectivity^b(%)
1	H	H	99	99
2	CH₃	H	99	99
3	CH₃O	H	99	99
4	Br	H	80	99
5	NO₂	H	75	99
6	CF₃	H	70	99
7	H	CH₃	40	99

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