"Mobile Domains"-Holding Polymer Reactors And Tunable Tandem Catalysis

Catalysis is the cornerstone of the modern chemical industry.It plays an indispensable role in the modern chemical industry.It is an important factor restricting the development of the modern chemical industry.The realization of intelligent and controllable catalytic processes is a major scientific and technical problem that the industry needs to solve urgently.In actual industrial production,most catalysis processes involve many reaction intermediates and complex reaction steps.Therefore,the treatment of these reactions usually requires control of the catalysis process in order to achieve high selectivity catalysis,controllable and self-adjusting catalysis process,The required catalytic process such as substrate self-classification catalysis.However,due to the lack of simple and effective catalytic reactor design and research,it is difficult to rely on current catalyst design and production technology to achieve a fine,controllable and adjustable catalytic process.Therefore,in this paper,the following researches have been done on the design and synthesis of intelligently modifiable and controllable tandem catalytic reactors:In the first part of this article,we designed a double-layered polymer catalytic reactor with self-controlled tandem catalytic capability to achieve a tunable tandem catalytic process.Each layer is independently responsible for a process of tandem catalytic.The first layer of the polymer reactor is a shape-memory temperature-sensitive layer with "mobile domains".The opening and closing of the reactor channels are due to the fluidity of the polymer molecular side chains.At low temperature,the molecular side chains are in "frozen" state,so it can prevent the reaction substrate from entering the reactor.At high temperature,the fluidity of the shape memory polymer side chains are enhanced,and the reactor channels are "open" to participate in the reaction The substrate can enter the reactor and contact with acid sites,thereby hydrolyzing to generate intermediate products.The second layer of the reactor is a molecularly imprinted layer encapsulated with metal nanoparticles,and the imprinting template is an intermediate product,so that only the intermediate product of the reaction can enter the imprinting layer for subsequent reactions.In this way,the tandem catalysis process of the reactants is realized,which provides an opportunity to realize a tunable catalytic reaction process.On the basis of the above design,we also combined molecular imprinting technology and "mobile domains" shape memory polymer to develop a "selective / non-selective" commutation tandem catalytic reactor.The reactor is a thermosensitive network structure with molecular imprinting introduced into the shape memory polymer.We used two catalytic substrates(NPA and BNPC)to conduct catalytic test comparison.At low temperature,the imprinted structure only allows the template molecule NPA to enter the reactor(but BNPC cannot enter the reactor),so it can effectively carry out the hydrolysis-reduction reaction after contact with the acid sites and the metal nanoparticles of the capsule.In contrast,at high temperatures,the "mobile domains" of the reactor destroys the imprinting channels,and the reactor assumes a "non-selective" state.At this time,both NPA and BNPC can enter the reactor for hydrolysis-reduction reaction.In this way,through the use of temperature as a means of regulation,a “selective / non-selective” commutation tandem catalysis process is realized.In the third part of this article,on the basis of the first two parts,two molecularly imprinted polymer layers are introduced to achieve the tunable tandem reaction process.The aim is to effectively separate the two processes of hydrolysis and reduction so as to control the catalytic reaction and make it easier to operate.The reactor is composed of two layers,the first layer is an acid layer,the second layer is an intermediate imprinted molecularly imprinted layer,and metal nanoparticles are embedded in the imprinted layer.In this way,the two processes of substrate hydrolysis and reduction are carried out separately in two separate layers,therefore,while allowing the switching between "selective" and "non-selective",it is more conducive to controlling and adjusting the series catalytic process.Through the above research contents,we have enriched the types of tandem catalysts,provided more opportunities in the field of tandem catalysis,and made the adjustment of complex reaction processes involving multiple components possible.