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Nanjing University Liu Zhen's research team reported a new template docking surface blotting strategy (RMTD-SI) based on reverse phase microemulsion, which is used to design and prepare molecularly imprinted nanoenzymes with open structures, so that it has the ability to capture substrates freely and is used for catalytic ligation of ssDNA. The prepared molecularly imprinted nanoenzymes can significantly increase the rate of catalytic reactions and exhibit good substrate selectivity. In addition, this molecularly blotting nanoenzyme can further catalyze the ssDNA having a sequence that is exactly matched to the blotting cavity to the product that forms a longer sequence.
Figure 1 (a) Principles and flowchart of template docking surface blotting (RMTD-SI) strategy based on reverse phase microemulsion. (b) Schematic diagram of the catalytic mechanism of molecularly imprinted nanoenzymes prepared by the RMTD-SI strategy.
natural enzyme, as a highly specific biocatalyst , can increase the reaction rate by several orders of magnitude by enzymatic reaction under mild conditions, thereby efficiently and specifically catalyzing the production of products. However, natural enzymes have disadvantages such as poor in vitro stability, difficulty in large-scale preparation and difficulty in reusing, which prompted researchers to develop artificial enzymes. As a new artificial enzyme, nanoenzymes have obvious advantages over natural enzymes, such as higher catalytic activity, better controllability, simple preparation, and easy use. They are expected to become a substitute for natural enzymes, which has attracted widespread attention in the past decade.
molecularly imprinted polymer (MIP) can be used as a novel nanoenzyme due to its good specificity and high affinity. Early molecularly imprinted nanoenzymes used transition state analogs (TSAs) as templates to generate active sites, providing a new way to prepare nanoenzymes. In the presence of a blotting cavity, the reactants can be induced to form a transition state, reducing the activation energy of the reactants, thereby increasing the reaction rate. However, blotting using transition state analogs depends on the accurate grasp of the transition state and transition state analog structure, and the structure of transition state analogs will vary greatly with the reaction substrate. These bring great challenges to the preparation of molecular imprinted nanozymes and seriously limit the development and application of molecular imprinted nanozymes.
To overcome the above problems, Liu Zhen’s research team first proposed a new catalytic strategy - affinity aggregation enhancement coupling (AGEC) in its previous work (Journal of Materials Chemistry B, 2022, DOI: 10.1039/D1TB02325J), which specifically recognizes the reaction substrate using the imprinted cavity and pulls the reaction groups of different substrates closer, increasing the collision probability of active groups to speed up the reaction speed. At the same time, combined with the strategy of temperature cyclic amplification (TCA), the hydrogen bonding effect of the blot cavity is controlled through temperature changes to avoid product inhibition effect. The team has verified the feasibility of this strategy by using the target product as a blotting template. However, since the pores of the mesoporous material are located inside the material, which is not conducive to the synthesis and catalytic reaction of macromolecules, it is necessary to design a new nanostructure for extended application of this catalytic strategy.
Based on the above questions, Liu Zhen’s research team developed a new strategy called “Template Docking Surface Imprinting (RMTD-SI) based on reverse phase microemulsion” to design and prepare molecular blotting nanoenzymes with open structures, giving them the ability to capture substrates freely for catalytic ligation of ssDNA. The research team conducted in-depth research on the properties and catalytic behavior of this novel molecularly imprinted nanoenzyme and explored its possible mechanism. Using the AGEC strategy, it was proved that the molecular imprinted nanoparticle can act as a nanoenzyme, catalyzing the ligation of ssDNA substrates, showing good catalytic activity and substrate selectivity.In addition, unlike previously reported molecularly imprinted nanoenzymes based on mesoporous materials, the molecularly imprinted nanoenzymes reported in this study can further catalyze the ssDNA with sequences that are perfectly matched to the blotting cavity to other ssDNA substrates, forming products of longer sequences, but lose selectivity for other substrates. Through mechanism analysis, this may be due to the free capture ability of substrates brought by its open structure. Therefore, this study not only provides new strategies for the design and preparation of molecularly imprinted nanoenzymes, but also provides new insights into the catalytic behavior of molecularly imprinted nanoenzymes.
Paper information
Molecularly Imprinted Nanozymes with Free Substrate Access for Catalyzing the Ligation of ssDNA Sequences
Zhanchen Guo+, Qi Luo+, Prof. Dr. Zhen Liu*
This article is included in the special collection of "European Chemistry" "Nanjing University's 120th Anniversary" of Nanjing University.
Chemistry – A European Journal
DOI: 10.1002/chem.202202052
Chemistry – A European Journal
《European Chemistry is the official journal of the European Chemistry Association (Chemistry Europe) and is published by Wiley–VCH. As an international platform for outstanding scientific publication, it publishes the best quality original basic research and special reviews in various chemistry fields.
