Post-synthetic modification of zirconium metal-organic frameworks by catalyst-free aza-Michael additions

被引：18
|
作者：
Hamzah, Harina Amer [1 ]
Crickmore, Tom S. [1 ]
Rixson, Daniel [1 ]
Burrows, Andrew D. [1 ]
机构：
[1] Univ Bath, Dept Chem, Bath BA2 7AY, Avon, England
来源：
DALTON TRANSACTIONS | 2018年 / 47卷 / 41期
基金：
英国工程与自然科学研究理事会;
关键词：
UIO-66; CO2; FUNCTIONALIZATION; REMOVAL; CAPTURE; CHANNELS; DEFECTS;
D O I：
10.1039/c8dt03312a
中图分类号：
O61 [无机化学];
学科分类号：
070301 ; 081704 ;
摘要：
The reactions of the zirconium MOF [Zr6O4(OH)(4)(bdc-NH2)(6)] (UiO-66-NH2, bdc-NH2 = 2-amino-1,4-benzenedicarboxylate) with the Michael acceptors acrylonitrile (CH2=CHCN), acrylic acid (CH2=CHCO2H), methyl acrylate (CH2=CHCO2Me) and methyl vinyl ketone (CH2=CHC(O)Me) led to post-synthetic modification of the MOF through C-N bond formation without loss of crystallinity. The reactions with acrylonitrile and acrylic acid go to completion, yielding [Zr6O4(OH)(4)(bdc-NHCH2CH2CN)(6)] (UiO-66-AN, 1) and [Zr6O4(OH)(4)(bdc-NHCH2CH2CO2H)(6)] (UiO-66-AA, 2) respectively, whereas those with methyl acrylate and methyl vinyl ketone are incomplete, yielding [Zr6O4(OH)(4)(bdc-NH2)(0.66)(bdc-NHCH2CH2CO2Me)(5.34)] (UiO-66-MA, 3) and [Zr6O4(OH)(4)(bdc-NH2)(2.76)(bdc-NHCH2CH2C(O)Me)(3.24)] (UiO-66-MVK, 4), respectively. The acrylonitrile-modified MOF UiO-66-AN undergoes further reaction with sodium azide in the presence of zinc(II) chloride in n-butanol to form the tetrazolate-modified MOF [Zr6O4(OH)(4)(bdc-NHCH2CH2CN)(4.74)(bdc-NHCH2CH2CN4H)(1.26)] (UiO-66-TZ, 5).
引用
收藏
页码：14491 / 14496
页数：6
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