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基于剛性吡嗪四羧酸和柔性吡嗪四咪唑配體的金屬有機(jī)框架的合成及性能研究

發(fā)布時(shí)間:2018-09-13 14:56
【摘要】:金屬-有機(jī)框架(MOFs)是金屬離子和有機(jī)配體通過(guò)配位鍵組裝而成,作為新一代的高孔隙度的分子晶體材料在最近的二十多年中被廣泛的研究與報(bào)道,這是由于它們迷人的晶體結(jié)構(gòu)與各種各樣的潛在應(yīng)用,如氣體的存儲(chǔ)與分離、催化、磁性、熒光、化學(xué)傳感等。本文通過(guò)設(shè)計(jì)合成了新的氮雜環(huán)有機(jī)配體,通過(guò)水熱法合成了新的金屬-有機(jī)框架配合物,并對(duì)其結(jié)構(gòu)和性能進(jìn)行了表征與測(cè)試。具體內(nèi)容分為以下幾個(gè)部分:第一部分;介紹金屬-有機(jī)框架的發(fā)展背景、合成方法、影響因素、性能測(cè)試等。第二部分;設(shè)計(jì)并合成了剛性的2,3,5,6-四(4-羧基苯基)吡嗪配體,和不同的金屬鹽在水熱條件下合成了六個(gè)多孔的金屬-有機(jī)框架材料:{Cd(L1)×2H_2O}n(1),{Pb_2(L1)}n(2),{La(L1)×H_2O×2.7 H_2O}n(3),{Sr_3(L1)2×6H_2O×2.6 H_2O}n(4),{Ce(L1)×4H_2O×H_2O}n(5),{Mn_2(L1)}n(6),并對(duì)其結(jié)構(gòu)進(jìn)行了表征。測(cè)試了配合物的熱重、固態(tài)紫外、固態(tài)熒光、氣體吸附、電化學(xué)催化析氫等性能。配合物表現(xiàn)出良好的熱穩(wěn)定性,分解溫度都能達(dá)到450°C左右。配合物1和4相對(duì)于L1配體展現(xiàn)出明顯的熒光增強(qiáng)性能,可作為潛在的熒光材料。氣體吸附實(shí)驗(yàn)發(fā)現(xiàn)配合物3和6展現(xiàn)出非常好的N2吸附性能,并對(duì)配合物6做了H_2的吸附測(cè)試。配合物2和5展現(xiàn)出一定的電化學(xué)析氫性能。第三部分;設(shè)計(jì)并合成了柔性的四齒咪唑配體,隨后與不同的羧酸組裝了四個(gè)金屬-有機(jī)框架配合物:{Co(L2)A}n(L2=2,3,5,6-四(4-亞甲基-1-咪唑苯基)吡嗪A=5-硝基間苯二甲酸)(7),{Co(L2)·2H_2O}n(8),{Co(L2)B}n(B=4,4`-二苯醚二甲酸)(9),{Mn_2(L2)C_2}n(C=1,4萘二甲酸)(10)。通過(guò)單晶X-射線衍射對(duì)其結(jié)構(gòu)進(jìn)行了確認(rèn),并通過(guò)P-XRD,紅外對(duì)結(jié)構(gòu)進(jìn)行了表征。測(cè)試了部分化合物的性能,配合物8展現(xiàn)出良好的催化析氫性能。第四部分;全文總結(jié)。
[Abstract]:Metal-organic framework (MOFs) is composed of metal ions and organic ligands assembled by coordination bonds. As a new generation of molecular crystal materials with high porosity, (MOFs) has been widely studied and reported in recent twenty years. This is due to their fascinating crystal structure and various potential applications, such as gas storage and separation, catalysis, magnetism, fluorescence, chemical sensing, etc. In this paper, a new organic ligand with heterocyclic nitrogen was designed and synthesized, and a new metal-organic frame complex was synthesized by hydrothermal method. Its structure and properties were characterized and tested. The content is divided into the following parts: the first part introduces the development background of metal-organic framework, synthesis methods, influencing factors, performance testing and so on. 絎簩閮ㄥ垎;璁捐騫跺悎鎴愪簡(jiǎn)鍒氭,

本文編號(hào):2241501

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