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Design,Synthesis And Application Of Functional Coordination Polymer For Environmental Protection

Posted on:2019-10-03Degree:DoctorType:Dissertation
Country:ChinaCandidate:L F LiangFull Text:PDF
GTID:1361330551956969Subject:Inorganic Chemistry
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With the rapid development of the society,the protection of ecological environment has gradually become a hot topic in the world,among them water pollution and air pollution are the problems to be solved urgently.Adsorption method is the main method of treating wastewater and waste gas in today’s society,but traditional adsorbents usually face challenges like low adsorption quantity,the poor selectivity,not easy to regenerate.So it is a pressing task to look for new adsorbents with high efficiency and low energy consumption for water and air protection.Coordination polymer is a class of material composed of organic ligands and metal ions or metal clusters,which are self-assembled by coordination bond.With characteristics like novel structure,high specific surface area and porosity,and regulatory pore environment,this kind of material displays a good application prospect in the ecological environmental protection,catalysis,molecular detection and drug delivery etc.The main research contents and test results are listed as follows:Chapter 1 is the introduction part mainly reviews the development of coordination chemistry and the development direction of future research,discusses the coordination polymer functional method and their uses in ecological environment protection,and finally illustrates this topic research background and its significance.Chapter 2 mainly describes the design and synthesis of a sulfur functionalized coordination polymer FJI-H12 and its application in mercury adsorption.The content is divided into two parts.In the first part,tridentate ligand Tizt and cobalt thiocyanate was choosed to construct the coordination polymer FJI-H12.FJI-H12 has a two-fold interpenetration and each fold is connected by a 3,4-connected octahedral cages,in which each cobalt vertex is coordinated with two nitrogen atoms of thiocyanate group and and four nitrogen atoms from four different ligands.The sulfur atoms of thiocyanate groups are pointing in the direction of the cavity and can be used for the adsorption of mercury ion in aqueous solution.Further study on its mercury adsorption capacity find out that FJI-H12 has good mercury adsorption properties.The microcrystals of FJI-H12 can be synthesized in large scale under room temperature in the system of ethanol and water,and the FJI-H12 can be regenerated easily with potassium thiocyanate solution.Chapter 3 introduces a method for the introduction of ultrasmall metal sulfide nanoparticles into the cavity of a coordination polymer.A reported very stable mesoporous coordination polymer material,MIL-1 O1(Cr)was choosed as the carrier.Indium sulfide was choosed because of its good water stability and strong interaction with mercury ions.The synthesis process is divided into two steps:the first step is to introduce the trivalent indium ions into the cavity of MIL-101 by double solvent method and the second step is to carry out the gas-solid reaction in MIL-101 of the trivalent indium ion with hydrogen sulfide gas,and assemble the sulfide nanoparticles in the cavity of MIL-101.The prepared In2S3 @MIL-101 composite material can effectively remove 99.95%Hg in wastewater within 1 minute,and the saturated adsorption capacity is as high as 518.2mg g-1.In addition,pH and different interfering ions almost have no influence on the mercury removal performance of In2S3 @MIL-101.Chapter 4 mainly describes the design and synthesis of the coordination polymer FJI-H14 with high density polar atoms and its application in carbon dioxide adsorption.Under hydrothermal conditions,H2BTTA ligand with high proportion of nitrogen and oxygen atoms and bivalent copper ion were designed to assemble coordination polymer FJI-H14.The total concentration of carbon dioxide philic sites of FJI-H14 including unsaturated coordinated Cu atoms and free N atoms,is 9.2 mol L-1,which is higher than most of those reported in literature with high carbon dioxide adsorption.The material has good water stability,thermal stability,acid and alkali stability,and can be easily prepared in large scale.FJI-H14 has a high carbon dioxide adsorption and can be resued without performace loss.Both the experiment and calculation show that the adsorption is derived from the interaction between various kinds of active sites and carbon dioxide molecules.In addition,FJI-H14 can effectively catalyze the conversion of carbon dioxide into useful carbonate in the industrial waste gas emission system under mild conditions.These researches enrich the contents of functional coordination polymers,provide a theoretical basis and experimental models in the field of selective adsorption of heavy metal ions,small gas molecules etc.
Keywords/Search Tags:Functional Coordination Polymer, Ecological Environment Protection, Mercury Pollution, Carbon Dioxide Adsorption
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