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The Catalytic Tandem Click/Alkynylation Reaction And Glucose Sensing Properties Of Coordination Polymer Constructed By Multidentate Nitrogen Heterocyclic Ligands

Posted on:2020-06-09Degree:MasterType:Thesis
Country:ChinaCandidate:X Q GuoFull Text:PDF
GTID:2381330575455379Subject:Inorganic Chemistry
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Coordination polymers?CPs?composing of metal ions/metal clusters and functionalized organic ligands are a class of crystalline materials with a well-defined structure.MOFs have the following four distinct features:?i?special porosity and adjustable pore size leading to a diversity of porous structures;?ii?Structural design is achieved by considering the preferred topology;?iii?Post-synthesis modification?PSM?of CPs is one of the powerful tools for changing the accessibility and reactivity within pores and altering the electronic and spatial characteristics of active sites;?iv?The active species are embedded in the CPs backbone which may be result in differently distributed functional sites within the pores.These unique features have led to extensive research on CPs in many applications,such as:catalysis,Sensing,gas adsorption and separation,and energy storage.In recent years,many studies have focused on CPs as heterogeneous catalysts to catalyze organic reactions,such as Henry reaction,transesterification reaction,cycloaddition reaction,Michael addition,one-pot cascade reaction.Knoevenagel condensation,aldol condensation,Suzuki coupling reaction,and so on.With its unique pore structure,modification and high specific surface area,it combines the advantages of homogeneous and heterogeneous catalysts and exhibits excellent catalytic performance.On the other hand,CPs are also widely used in the field of electrochemical biosensing.Based on the above discussion,The research contents of this thesis include:1)Designing and synthesizing a novel Cu?I?coordination polymer as a heterogeneous catalyst to catalyze a three-component click/Alkynylation reaction to form a completely substituted triazole skeleton product,and exploring the relationship between the catalytic performance and structures.2)designing and synthesizing a new type of glucose sensor and then studing its electrocatalytic performance for glucose.At the same time,the selectivity and stability of the coordination polymer as a glucose sensor are also investigated.The details are as follows:1.To expand CPs as solid catalysts to selectively catalyze tandem Click/Alkynylation reaction for their fully substituted triazoles skeletons,two Cu?I?-based CPs?CuI-CPs?,[CuBr?aas-TPB?]n?1?and[Cu3I3?aas-TPB?2]n?2??TPB=N,N,N-tri?3-pyridinyl?-1,3,5-benzenetricarboxamine?have been prepared.Because of the template effect of anions?Br-and I-?,the structure of compounds is regulated under solvothermal conditions.CPs 1 exhibited one-dimensional?1D?chain,while the double strands framework with Cu3I3 cluster platform was observed in 2.In addition,the different product selectivity of catalyzing terminal alkynes,benzyl azide and bromoalkyne to synthesize triazoles skeletons has been caused by the significantly structural diversity of CPs 1 and CPs 2.The unique Cu3I3 structure of CPs 2 can effectively promote the three-component Click/Alkynylation reaction.As a result,CPs 2 can be a candidate for outstanding catalyst for sequential Click/Alkynylation cycloaddition,while CPs 1 can efficiently catalyze the generation of click products.2.We synthesized a divalent cobalt coordination polymer CoII-CP?3?under solvothermalconditionsusingaligandcontainingN?4,5-bis?tetrazol-5-yl?imidazole?.Single crystal X-rays indicate that the coordination polymer CPs 3 shows an"herringbone"one-dimensional chain structure.According to its structural characteristics,we applied CPs 3 to the detection of glucose.The experimental results show that the coordination polymer has a low detection line for glucose detection and a fast response,and is a novel detection glucose sensor.
Keywords/Search Tags:Coordination polymer, synergistic catalysis, sensor, tandem click/Alkynylation reaction, glucose detection
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