Thermosensitive Smart Catalytic Reactors And Their Functional Catalysis

The rapid development of the chemical industry is inseparable from the advancement of catalysts,especially the establishment of petroleum-based petrochemicals?including rubber,plastics,fibers,pesticides and basic organic synthesis industries?.The use of catalysts has greatly changed the production and life of human beings,and almost created an era of artificial“everything”.The design of the catalyst has made the catalytic science an unprecedented leap.Among them,the"soft"nature of polymer and the"arbitrary"stacking of molecular segments can be used as a carrier for metal nanoparticles to develop new concepts and new functional catalytic reactors,which has made the functional catalyst and catalytic concept unprecedentedly improved.Although the field is progressing relatively fast,it rarely involves complex reactions such as series and classification,and it is unable to meet the needs of the development of controllable and modulating catalysis.In view of the main problems in the field of catalytic reactor,new conceptual reactors,such as series reactor and self-classification reactor,were developed in order to provide some ideas for the development of new conceptual intelligent catalysts.In the first part,we first designed the acid-base nucleocapsid thermosensitive intelligent polymer reactor:study the structure of the multi-compartment cell,prepare a three layers core-shell polymer reactor.The Preparation of basic core layer is by2-methylallylamine,2-acrylamido-2methylpropanesulfonic acid?AMPS?as acidic shell,and nitrogen isopropyl acrylamide?PNIPAM?as intelligent response layer.It is found that the the intermediate channel of the synthesized reactor is“opened”by the temperature sensitive layer under low temperature conditions,,and the substrate can be sequentially contacted with acidic and alkaline sites to realize series catalysis;on the contrary,with the increase of temperature,The hydrophobic action of PNIPAM causes the intermediate channel to close,resulting in a series reaction that does not proceed smoothly?only the first half of the reaction can be performed?.We obtained the basic morphology and size by SEM and TEM.The preparation of the three-layer structure was confirmed by particle size analysis.The phase transition of the synthesis reactor at about 32? was confirmed by DLS,and the electrochemical reaction confirmed the synthesis reaction.The device has a temperature response function.In the second part,we designed a new concept reactor with a graded response self-classification catalytic function:studying the self-assembly of protein macromolecules,usingacombinationoftwointeractions,from poly-2-trifluoromethacrylic acid?PTFMA?Poly-3-buten-1-ol and polyvinylimidazole?PVI?copolymerize to form a temperature sensitive layer.As a functional carrier of Ag nanoparticles,polyacrylamide?PAM?is used as an inert matrix layer.It is found that the interaction between hydrogen bonding and electrostatic interaction is different,and its order dissociation enables the reactor to achieve anti-self-classification catalysis.The study found that the reactor has a Thermosensitive recognition behavior at 45?and 65?;the UV-catalyzed analysis of the small molecule substrate p-nitrophenol?NPh?and the macromolecular substrate methylene blue?MB?:reactor At low temperatures,the catalytic efficiency of both substrates is only about 15%,while the catalytic efficiency of Nph reaches 70%at medium temperature,and the catalytic efficiency for MB is still not high?about 25%?when the temperature reaches65?.At the same time,the catalytic efficiency of both substrates reached more than80%.In the third part,we also prepared a temperature sensitive molecularly imprinted reactor.The series catalysis of hydrolysis and reduction of p-nitrophenyl acetate?NPA?was achieved through the synergistic effect of two recognition functions.The temperature sensitive layer is formed by copolymerization of NIPAM and AMPS,and the molecular imprinting is to imprint the p-nitrophenol?NPh?and embed Ag nanoparticles.The SEM,TEM and SPR were used to analyze the morphology of the reactor.The successful encapsulation of Ag nanoparticles was confirmed,and the successful preparation of the molecularly imprinted layer was preliminarily proved.The infrared contrast and TPD analysis before and after the template elution were further analyzed.Molecularly imprinted layer;the phase change behavior of the temperature sensitive layer was deeply analyzed by DLS and electrochemical workstation;BET analysis of the reactor was also carried out,and it was found that the molecularly imprinted polymer reactor had a large specific surface area and specific volume(142.6 m²g^-1,61.2?L g^-1);Finally,the substrate was subjected to UV catalytic analysis to determine that the reactor is a smart and controllable catalytic function that realizes the series reaction through the synergy of two layers.From the above work,we systematically studied the design of functional polymer reactors and various influencing factors and functional catalysis.The regulation mechanism of the reactor was explained at the molecular level,which provided the necessary experimental data for the development of new series-classified intelligent catalysts.And the foundation to create the necessary conditions for the design of the new concept functional catalyst.