Inspired by nature,precise spatial organization of enzyme cascades of interest is crucial to the improvement of catalytic performance.Herein,DNA scaffolds were introduced to construct a toolkit for versatile immobilization of enzyme pairs on dextran-coated magnetic nanoparticles(MNPs).After the glucose oxidase(GOx)and horseradish peroxidase(HRP)pair was immobilized through random cova-lent,DNA-directed and DNA tile-directed strategies,the immobilized GOx/HRP pair on the MNP-based carrier assembled with DNA tile(TD@MNPs)exhibited the highest activity due to rational spatial organization and less conformational change of constituent enzymes.With a decrease in interenzyme distance on TD@MNPs,furthermore,the catalytic efficiency of the HRP/GOx pair increased further for both substrates,2,2'-azinobis(3-ethyl-benzthiazoline-6-sulfonate)(ABTS)and 3,3',5,5'-tetramethyl benzidine(TMB).As the assembled HRP was closer to the carrier surface,the catalytic efficiency of the GOx/HRP pair increased by 6.2-fold for positively charged TMB and only by 62％for negatively charged ABTS compared with the free GOx/HRP pair.Moreover,a reversal of catalytic efficiency was found after the GOx/HRP pair was assembled on a positively charged carrier(TD@pMNPs).This research demonstrated that MNP-based car-riers had the potential to become a versatile toolkit for shedding an insight into catalytic performance and the development of new biocatalysts.

Xinshuang Chu;Qinghong Shi

Deportment of Biochemical Engineering,School of Chemical Engineering and Technology,Tianjin University,Tianjin 300350,China;Key Laboratory of Systems Bioengineering and Frontiers Science Center for Synthetic Biology(Ministry of Education),Tianjin University,Tianjin 300350,China

中国化学（英文版）

[1]Xinshuang Chu;Qinghong Shi-.Versatile Magnetic Nanoparticles for Spatially Organized Assemblies of Enzyme Cascades:A Comprehensive Investigation of Catalytic Performance)[J].中国化学（英文版）,2022(12):1437-1446

Organized,interenzyme,benzthiazoline,benzidine,pMNPs,biocatalysts

Versatile,Magnetic,Nanoparticles,Spatially,Assemblies,Enzyme,Cascades,Comprehensive,Investigation,Catalytic,Performance,Inspired,by,nature,precise,spatial,organization,cascades,interest,crucial,improvement,catalytic,performance,Herein,scaffolds,were,introduced,construct,toolkit,versatile,immobilization,pairs,dextran,coated,magnetic,nanoparticles,After,glucose,GOx,horseradish,peroxidase,HRP,was,immobilized,through,random,cova,lent,directed,strategies,carrier,assembled,TD,exhibited,highest,activity,due,rational,less,conformational,change,constituent,enzymes,With,decrease,distance,furthermore,efficiency,increased,both,substrates,azinobis,sulfonate,ABTS,tetramethyl,TMB,closer,surface,positively,charged,only,negatively,compared,free,Moreover,reversal,found,after,This,research,demonstrated,that,riers,had,potential,become,shedding,insight,into,development,new

0.502602