Research On The Preparation And Application Of Nano-adsorbent Materials Based On Typical Pollutants In The Water Environment Of The Three Gorges Reservoir Are

Since the L-proline-catalyzed intermolecular asymmetric aldol reaction and the secondary amines-catalyzed asymmetric Diels-Alder reaction opened the prelude to the study of asymmetric reactions catalyzed by small organic molecule catalysts,organocatalysis has witnessed the rapid development since 2000 and so far is still in the ascendant.As a relatively unique direction of organic catalysis,N-Heterocyclic carbene（NHC）is widely used in the construction of various chemical bonds and has developed many new chemical reaction modes.A series of chiral compound fragments with important application value and pharmacodynamic structures with good biological activity could be synthesized through these new chemical reaction strategies,which conversely broadened the application scope of asymmetric reactions realized by NHC catalysts.In addition,compounds containing carbonyl groups are a class of functional substrates that are easily available and easy to be modified and derivatized to afford many desired molecules with certain physiological activities through practical chemical modifications of these functional substrates.These target compounds are widely used in th fields of materials,chemistry and chemical industry,medicine and pesticides.However,there have certain difficulties in the study of long-distance carbon-functionalization of carbonyl compounds,especially for obtaining some target molecules with good enantioselectivity control,which brings great challenges to chemists at the same time and also is hot issues and difficulties of the research in this field.This dissertation mainly focuses on exploring theδ-carbon functionalization of carbonyl compounds to seek a simple,highly efficient and easy-to-operate chemical reaction method for constructing a series of small candidate molecules with potential biological activities.Through the evaluation of biological activity tests,we hope that leading structures with good biological activities will be found from many candidate compounds,which will provide a technical and theoretical support for the sustainable development of high-efficiency and low-risk green small-molecule pesticides.The main contents of this research are summarized as follows:1.We disclosed a chemo-selective cascade cycloaddition reaction promoted by simple and readily available Na OH.Through this strategy,the D-A cyclopropyl esters could be ring-opening to in situ generateα,β-unsaturated carboxylic ester.Theα,β-unsaturated carboxylic ester is activated as the nucleophile to react withα,β-unsaturated imines in highly chemo-selective manners.25 Cyclopenta[c]pyridine derivatives are afforded as the final products in up to quantitative yields through the cascade cycloaddition process.The structures of these compounds were confirmed by X-ray and characterized by ¹H NMR,¹³C NMR and HR-MS.The in vitro antibacterial activities of model compounds against Xanthomonas oryzae pv.oryzae（abbr.as Xoo）,Xanthomonas axonopodis pv.citri（abbr.as Xac）and Pseudomonas syringae pv.actinidiae（abbr.as Psa）were tested by turbidity method,respectively.These test results showed that most of the compounds exhibited promising inhibitory activities against three phytopathogenic bacteria at the tested concentration.Specifically speaking,the inhibitory rates of compound 2-3e against Xoo at the concentration of100 and 50μg/m L were 63.1%and 23.9%,respectively,which were slightly better than that of the control agent.Compound 2-3d exhibited a inhibition rate of 47.0%at the concentration of 100μg/m L against Xac However,this compound showed nearly no inhibitory activities against Xac when the tested concentration was decreased to 50μg/m L.The inhibitory activities of compounds 2-3c and 2-3q against Psa at the concentration of 100μg/m L were 54.1%and 50.2%,respectively,which was slightly better than the positive control.The multi-functional cyclopenta[c]pyridine products obtained from our method exhibit encouraging anti-bacterial activities with potential applications in the development of new green pesticides.In addition,the bioactivity of compounds against tobacco mosaic virus（abbr.as TMV）was tested by the half leaf spot method.The test results indicated the curative activities of compounds 2-3a,2-3p and 2-3r against tobacco mosaic virus at a concentration of 500μg/m L were 48.2%,47.5%and 47.9%,respectively,which are comparable to the activities of chitosan oligosaccharide（abbr.as COS）but lower than that of ningnanmycin（abbr.as NNM）.The protective activities of compound 2-3b against TMV at this concentration was68.6%,which was comparable to that of COS and slightly better than that of NNM.2.Based on the previous research work,we have developed a chemo-and diastereo-selective[3+2]cycloaddition between Donor-Acceptor cyclopropanes and substituted 3-vinyl indoles.Green,inexpensive,and readily available Na OH was used as the sole catalyst to promote this transformation.Structurally sophisticated spiro[cyclopentane-1,3’-indoline]derivatives bearing up to three adjacent chiral centers were afforded as the final products in generally good to excellent yields as single diastereomers.The structures of these spiro[cyclopentane-1,3’-indoline]compounds were characterized by ¹H NMR,¹³C NMR and HR-MS.The in vitro inhibitory activities of compounds against Phytophthora capsici and Colletotrichum capsici were tested by the mycelial growth rate method.The test results showed that the minority of compounds（e.g.,3-3a,3-3c and 3-3g）showed certain activities against Phytophthora capsici at the concentration of 50μg/m L.3.We have developed an eantionselective strategy for access to the chiral polycyclic epoxymethano-/epiminomethano-chromene molecules.Theδ-carbon of diunsaturated aldehyde is activated through the addition of a carbene to the aldehyde substrates under oxidative conditions.The diunsaturated acylazolium intermediate resulted from carbene-catalyzedδ-carbon activation react with 3-hydroxy pyrone or3-hydroxy-2-pyridone by means of asymmeteric D-A cycloaddition/lactonation process to afford a variety of epoxymethano-/epiminomethano-chromene analogues in generally good yield with excellent enatioselectivities.The structures of 29epoxymethano-/epiminomethano-chromene compounds were also characterized by¹H NMR,¹³C NMR,¹⁹F NMR and HR-MS.The in vitro inhibitory activities of the compounds against Phytophthora capsici and Colletotrichum capsici were tested by the mycelial growth rate method.When compared with the positive control agents,the test results indicated the minority of compounds exhibited a slightly promising fungicidal activities against the two phytopathogenic fungi in contrast to the two commercially used fungicidal agents-dithane z-78 and hymexazol（e.g.,4-3v,4-3w and 4-3aa,with inhibitory rates of 33.5%,36.0%and 37.0%,respectively）.