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Integration of enzyme immobilization and biomimetic catalysis in hierarchically porous metal-organic frameworks for multi-enzymatic cascade reactions

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Science China Chemistry 2022年第6期65卷 1122-1128页

作者： Shu-Fan Li Yan Chen Yi-Shu Wang Hui-Lin Mo Shuang-Quan Zang Henan Key Laboratory of Crystalline Molecular Functional Materials Henan International Joint Laboratory of Tumor Theranostical Cluster MaterialsGreen Catalysis CenterCollege of ChemistryZhengzhou UniversityZhengzhou450001China School of Chemistry and Chemical Engineering Nanjing University of Science and TechnologyNanjing210094China

Multiple enzymes-induced biological cascade catalysis is indispensable in biotechnology and industrial processes. Nevertheless,the drawbacks of most natural enzymes, including poor stability and recyclability and sensitivity to the environment, have hindered their broader application. Here, we report a facile strategy to prepare a biomimetic cascade reaction system by combining the advantages of enzyme immobilization and biomimetic catalysis in a one-pot reaction system based on the hierarchically porous metal-organic frameworks(HP-MOFs). The hierarchically porous zirconium-porphyrin-based MOF(HPPCN-222(Fe)) synthesized by modulator-induced strategy possessed tunable hierarchical porous and peroxidase-like activity,permitting them to act as not only an efficient immobilization matrix for glucose oxidase(GOx) but also peroxidase mimics to catalyze the cascade for glucose detection. A stable, anti-interference and reusable colorimetric biosensor for glucose detection was successfully established through GOx@HP-PCN-222(Fe) on the basis of the artificial tandem catalysis. Moreover, the GOx@HP-PCN-222(Fe)-fabricated electrode was available for glucose detection by electrochemical method. This work provides a potentially universal method to design functional multi-enzymatic cascade reaction systems by integrating the merits of enzyme encapsulation and biomimetic catalysis in HP-MOFs.

关键词： hierarchically porous metal-organic frameworks enzyme immobilization biomimetic catalysis multi-enzymatic cascade reactions

enzyme immobilization on a pH-responsive porous polymer membrane for enzymatic kinetics study

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Chinese Chemical Letters 2021年第10期32卷 3195-3198页

作者： Juan Qiao Lili Liu Ji Shen Li Qi Beijing National Laboratory of Molecular Sciences Key Laboratory of Analytical Chemistry for Living Bio-systemsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China College of Chemistry&Environmental Science Hebei UniversityBaoding 071002China

immobilization of enzymes onto carriers is a rapidly growing research area aimed at increasing the stability,reusability and enzymolysis efficiency of free *** this work,the role of phaseseparation and a pH-responsive"hairy"brush,which greatly affected the topography of porous polymer membrane enzyme reactors(PMER),was *** porous polymer membrane was fabricated by phase-separation of poly(styrene-co-maleic anhydride-acrylic acid)and poly(styrene-ethylene glycol).Notably,the topography and pores size of the PMER could be controlled by phase-separation and a pHresponsive"hairy"*** evaluating the enzymolysis efficiency of D-amino acid oxidase(DAAO)immobilized carrier(DAAO@PMER),a chiral ligand exchange capillary electrophoresis method was developed with D-methionine as the *** DAAO@PMER showed good reusability and stability after five continuous ***,comparing with free DAAO in solution,the DAAO@PMER exhibited a17.7-folds increase in catalytic velocity,which was attributed to its tailorable topography and pHresponsive *** poly(acrylic acid)moiety of poly(styrene-co-maleic anhydride-acrylic acid)as the pH-responsive"hairy"brush generated topography changing domains upon adjusting the buffer pH,which enable the enzymolysis efficiency of DAAO@PMER to be tuned based upon the well-defined architectures of the *** approach demonstrated that the topographical changes formed by phaseseparation and the pH-responsive"hairy"brush indeed made the proposed porous polymer membrane as suitable supports for enzyme immobilization and fitting for enzymolysis applications,achieving high catalytic performance.

关键词： enzyme immobilization Porous polymer membrane topography Phase separation pH-stimuli responsive hairy brush

POROUS SILICA NANO-TUBE AS HOST FOR enzyme immobilization

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China Particuology 2004年第6期2卷 270-273页

作者： Haomin Ding Lixiong Wen Jianfeng Chen Key Lab for Nanomaterials Ministry of EducationResearch Center of the Ministry of Education for High Gravity Engineering&TechnologyBeijing University of Chemical TechnologyBeijing 100029P.R.China

With their hollow morphology and large openings, the as-synthesized porous silica nano-tubes (NTPS), prepared through a sol-gel routine by using nano-sized needle-shaped CaCO3 particles as templates, were used as host for enzyme immobilization. Bioimmobilization study showed that enzyme molecules could not only be adsorbed on the external surface of NTPS but also entrapped in their inner hollow cores, leading to higher enzyme loading capacities of NTPS (more than 350 mg/g silica) in a shorter time, as compared to common porous silica (less than 50 mg/g) and most conventional mesoporous silica materials (less than 100 mg/g).

关键词： porous silica nano-tube nanosized CaCO_(3) lysozyme enzyme immobilization

A new inorganic-organic hybrid coordination polymer based on copper-substituted Keggin polyoxometalate used for enzyme immobilization

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A new inorganic-organic hybrid coordination polymer based on...

Visible light-driven oxidation of non-native substrate by laccase attached on Ru-based metal-organic frameworks

中国化学会第七届全国多酸化学学术研讨会

作者： Ying Lu Yue-Xian Zhang Jing Wang Fang Su Xiao-Jing Sang Zai-Ming Zhu Lan-Cui Zhang School of Chemistry and Chemical Engineering Liaoning Normal University

A new organic-inorganic hybrid coordination polymer containing organophosphine,inorganic phosphorus units and monovacant Keggin-type POM fragments,namely{H[(Cu(bipy))(PhPO)][PCuWO]?4HO}(1)(bipy=2,2’-bipyridine),was successfully synthesized and characterized by physico-chemical and spectroscopic *** crystal X-ray diffraction analysis reveals that compound 1 represents a new example formed by polyoxoanions and discrete transition metal-complex *** the crystal structure of compound 1,the adjacent[PWO]anions are bridged by the Cu(II) ions to give 1D inorganic polyanion chains,while the other existing 1D chains were constructed by discrete Cu(II)-organic complex cations ([Cu(bipy)(PhPO)]),the two kind of chains are connected with each other by electrostatic interactions to from a supramolecular ***,compound 1 was used as a support for immobilizing horseradish peroxidase (HRP)and showed excellent immobilizing *** maximum of HRP loading is 202.1 mg g under optimal ***,application of immobilized enzyme HRP/1 on the detection of HO was also discussed.

关键词： tungstophosphate coordination polymer crystal structure horseradish peroxidase enzyme immobilization

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Journal of Environmental Sciences 2024年第3期137卷 741-753页

作者： Wenguang Huang Wentao Zhang Guantongyi Chen Yun Chen Jun Ma Dawei Huang Qinzheng Zhaoc Bingdang Wu State Environmental Protection Key Laboratory of Environmental Pollution Health Risk Assessment South China Institute of Environmental SciencesMinistry of Ecology and Environment of PRCGuangzhou 510655China Tsinghua Shenzhen International Graduate School Tsinghua UniversityShenzhen 518055China School of Environmental Science and Engineering Suzhou University of Science and TechnologySuzhou 215002China Key Laboratory of Suzhou Sponge City Technology Suzhou 215002China

Light-induced electron transfer can broaden the substrate range of ***,the efficiency of photo-enzyme coupling is limited by the poor combination of photosensitizer or photocatalyst with ***,we prepared the nano-photocatalyst MIL-125-NH_(2)@Ru(bpy)by in site embedding ruthenium pyridine-diimine complex[Ru(bpy)_(3)^(2+)into metal organic frameworks MIL-125-NH_(2)and associated it with multicopper oxidase(MCO)*** to[Ru(bpy)_(3)]^(2+),the coupling efficiency of MIL-125-NH_(2)@Ru(bpy)_(3)for enzymatic oxygen reduction increased by 35.7%.A series of characterizations confirmed that the amino group of laccase formed chemical bonds with the surface defects or hydrophobic groups of MIL-125-NH_(2)@Ru(bpy)_(3).Consequently,the tight binding accelerated the quenching process and electron transfer between laccase and the immobilized ruthenium pyridine-diimine *** work would open an avenue for the synthesis of MOFs photocatalyst towards photo-enzyme coupling.

关键词： Laccase Light-driven biocatalysis Ruthenium photocatalyst Metal-organic frameworks enzyme immobilization

Dendrimer-induced synthesis of porous organosilica capsules for enzyme encapsulation

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Frontiers of Chemical Science and Engineering 2024年第4期18卷 41-48页

作者： Ziyi Chu Boyu Zhang Zhenhua Wu Jiaxu Zhang Yiran Cheng Xueying Wang Jiafu Shi Zhongyi Jiang School of Environmental Science&Engineering Tianjin UniversityTianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering Tianjin 300072China State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Organic matter-induced mineralization is a green and versatile method for synthesizing hybrid nanostructured materials,where the material properties are mainly influenced by the species of natural biomolecules,linear synthetic polymer,or small molecules,limiting their ***,we adopted dendrimer poly(amidoamine)(PAMAM)as the inducer to synthesize organosilica-PAMAM network(OSPN)capsules for mannose isomerase(MIase)encapsulation based on a hard-templating *** structure of OSPN capsules can be precisely regulated by adjusting the molecular weight and concentration of PAMAM,thereby demonstrating a substantial impact on the kinetic behavior of the MIase@OSPN *** MIase@OSPN system was used for catalytic production of mannose from Dfructose.A mannose yield of 22.24% was obtained,which is higher than that of MIase in organosilica network capsules and similar to that of the free *** overall catalytic efficiency(kcat/Km)of the MIase@OSPN system for the substrate D-fructose was up to 0.556 s^(-1)·mmol^(-1)·***,the MIase@OSPN system showed excellent stability and recyclability,maintaining more than 50% of the yield even after 12 cycles.

关键词： enzyme immobilization enzyme catalysis organosilica networks capsules sugar biosynthesis

Electrospun Poly(acrylonitrile-co-acrylic acid) Nanofibrous Membranes for Catalase immobilization:Effect of Porphyrin Filling on the enzyme Activity

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Chemical Research in Chinese Universities 2011年第2期27卷 339-344页

作者： KE Bei-bei WAN Ling-shu HUANG Xiao-jun XU Zhi-kang Key Laboratory of Macromolecular Synthesis and Functionalization Ministry of EducationDepartment of Polymer Science and Engineering Zhejiang University Hangzhou 310027 P. R. China

Porphyrin-filled nanofibrous membranes were facilely prepared by electrospinning of the mixtures of poly（acrylonitrile-co-acrylic acid）（PANCAA） and porphyrins. 5,10,15,20-Tetraphenylporphyrin（TPP） and its metal-loderivatives（ZnTPP and CuTPP） were studied as filling mediators for the immobilization of redox enzyme. Results indicate that the introduction of TPP, ZnTPP and CuTPP improves the retention activity of the immobilized catalase. Among these three porphyrins, the ZnTPP-filled PANCAA nanofibrous membrane exhibits an activity retention of 93%, which is an exciting improvement. This improvement is attributed to both the strong catalase-porphyrin affinity and the possible facilitated electron transfer induced by the porphyrin as evidenced by quartz crystal microbalance （QCM） and fluorescence spectroscopy studies.

关键词： enzyme immobilization Nanofibrous membrane Electrospinning Quartz crystal microbalance(QCM) Porphyrin

CATase-immobilized hydrogel platform molded by photo-enzyme coupling polymerization for effectively preventing postoperative abdominal adhesion

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中国科学:化学英文版 2023年第9期66卷 2664-2675页

作者： Min Hu Mingyue Shi Xia Wang Yujing Tang Dingze Zhou Kai Pan Qigang Wang School of Chemical Science and Engineering Tongji UniversityShanghai 200092China Translational Research Institute of Brain and Brain-Like Intelligence Shanghai Fourth People’s HospitalSchool of MedicineTongji UniversityShanghai 200434China

Redox homeostasis,which is regulated by enzymes acting as regulatory valves,is crucial for maintaining the proper functioning of biomolecules and a stable microenvironment for physiological processes by modulating the homeostasis of reactive oxygen species(ROS).Antioxidant enzymes in biocatalysis are used in the prevention or treatment of oxidative stress-related disease by counteracting the harmful effects of ***,designing a system that can efficiently immobilize antioxidant enzymes with high catalytic activity and stability is still *** by photo-biocatalysis,a novel and effective catalase(CATase)-immobilized hydrogel platform has been developed by the proposed photo-enzymatic coupled radical polymerization strategy of the visible light coupling with the porphyrin-centered *** higher catalytic stability and activity can therefore be achieved due to the preferential polymerization of CATase-immobilized hydrogel platform with a favorable three-dimensional network of enhanced coupling efficacy between light and *** mechanisms of free radical-initiated polymerization as well as the antioxidant cycle in the photo-CATase coupling system have been ***,the CATase-immobilized hydrogel platform affords an unprecedented antioxidant ability to scavenge ROS and provide an effective cellular protection mechanism against external oxidative ***,the CATase-immobilized hydrogel platform can effectively prevent peritoneal adhesion by reducing the expression of inflammatory ***,the novel CATase-immobilized hydrogel platform is a potential candidate for physical barriers that effectively prevent postoperative adhesion formation,offering a new anti-adhesion strategy for clinical applications.

关键词： photo-enzyme coupling polymerization enzyme immobilization antioxidative anti-inflammatory prevention abdominal adhesion

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Enhanced production of cytidine 5'-monophosphate using biocatalysis of di-enzymes immobilized on amino-functionalized sepharose

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Chinese Journal of Chemical Engineering 2023年第6期58卷 40-52页

作者： Xiaohong Zhou Wenfeng Zhou Wei Zhuang Chenjie Zhu Hanjie Ying Hongman Zhang School of Chemistry and Molecular Engineering Nanjing Tech UniversityNanjing 211816China State Key Laboratory of Materials-Oriented Chemical Engineering College of Biotechnology and Pharmaceutical EngineeringNational Engineering Technique Research Center for BiotechnologyNanjing Tech UniversityNanjing 211816China

Cytidine 5'-monophosphate(5'-CMP)is an essential nucleotide for *** this study,enhanced production of 5'-CMP was realized by the transformation of cytidine using co-immobilized di-enzymes,uridine-cytidine kinase(UCK)and acetate kinase(AcK).The immobilization yield of the enzyme had a clear correlation with the surface charges as zeta potential(ξ).Among them,ε-polylysinefunctionalized sepharose(SA-EPL,ξ=9.31 m V)showed high immobilization yield(78.8%),which was4.9-fold than that of nitrilotriacetic acid functionalized sepharose(SA-NTA,ξ=-12.6 m V).The residual activity of affinity co-immobilized enzyme(EPL-Ni/EPL@Ac K-UCK)was higher than 70.6%after recycled 10 ***,this study provides an effective approach for the production of 5'-CMP with the advantages of low adenosine 5'-triphosphate(ATP)consumption,reduced side reactions,and improved reusability by co-immobilized UCK and Ac K on the functionalized Sepharose.

关键词： Sepharose ε-Polylysine Dual-enzyme cascade Cytidine 5'-monophosphate enzyme immobilization