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A Pt/CeO_(2)Hybrid nanozyme with Stable Peroxidase Activity for the Detection of Acetylcholine

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Chemical Research in Chinese Universities 2024年第2期40卷 268-271页

作者： CUI Xulian MA Baofu PAN Hui XIA Yu LIU Li ZHAO Baofeng LIANG Zhen ZHANG Lihua ZHANG Yukui State Key Laboratory of Medical Proteomics Dalian Institute of Chemical PhysicsChinese Academy of ScienceDalian116023P.R.China The Research Center for Medical Genomics Key Laboratory of Medical Cell BiologyMinistry of EducationSchool of Life ScienceChina Medical UniversityShenyang110001P.R.China River Fisheries Research Institute Chinese Academy of Fishery SciencesGuangzhou510000P.R.China

Acetylcholine(ACh)is a common neurotransmitterl)that is secreted by cholinergic neurons[2]and is found mainly in the peripheral and central nervous systems.[3]ACh transmits nerve signals from presynaptic to postsynapt... 详细信息

关键词： Acetylcholine/choline nanozyme Hydrogen peroxide Alzheimer’s disease

NIR-switchable local hydrogen generation by tandem bimetallic MOFs nanocomposites for enhanced chemodynamic therapy

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Regenerative Biomaterials 2024年第1期3卷 58-68页

作者： Jun Zhong Xiang Zheng Yuan Wen Yuewei Li Jianting Zhang Ranjith Kumar Kankala Shibin Wang Aizheng Chen Institute of Biomaterials and Tissue Engineering Huaqiao UniversityXiamen 361021China Fujian Provincial Key Laboratory of Biochemical Technology Huaqiao UniversityXiamen 361021China Fujian Provincial Key Laboratory of Biomass Low-Carbon Conversion Huaqiao UniversityXiamen 361021China

The inadequate quantity of hydrogen peroxide(H_(2)O_(2))in cancer cells promptly results in the constrained success of chemodynamic therapy(CDT).Significant efforts made throughout the years;nevertheless,researchers are still facing the great challenge of designing a CDT agent and securing H_(2)O_(2) supply within the tumor cell.In this study,taking advantage of H_(2)O_(2) level maintenance mechanism in cancer cells,a nanozyme-based bimetallic metal-organic frameworks(MOFs)tandem reactor is fabricated to elevate intracellular H_(2)O_(2) levels,thereby enhancing CDT.In addition,under nearinfrared excitation,the upconversion nanoparticles(UCNPs)loaded into the MOFs can perform photocatalysis and generate hydrogen,which increases cellular susceptibility to radicals induced from H_(2)O_(2),inhibits cancer cell energy,causes DNA damages and induces tumor cell apoptosis,thus improving CDT therapeutic efficacy synergistically.The proposed nanozyme-based bimetallic MOFs-mediated CDT and UCNPs-mediated hydrogen therapy act as combined therapy with high efficacy and low toxicity.

关键词： chemodynamic therapy nanozyme bimetallic MOFs gas therapy

Bioinspired nanomaterials for the treatment of bacterial infections

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Nano Research 2024年第2期17卷 691-714页

作者： Xiaojing Ma Wenjing Tang Rong Yang Robert F.Smith School of Chemical&Biomolecular Engineering Cornell UniversityIthacaNY 14853USA

Infectious diseases pose a serious threat to global health.Although immunizations can control most viral infections,bacterial infections,particularly those caused by drug-resistant strains,continue to cause high rates of illness and death.Unfortunately,the creation of new antibiotics has come to a grinding halt in the last ten years.In response to this crisis,nanotechnology has emerged as a hopeful solution to tackle drug resistance and enhance treatment results.A large variety of biomimetic nanomaterials,termed nanozymes,have demonstrated strong antimicrobial efficacy.While the inherent toxicity of nanomaterials is a concern,recent studies have harnessed the stimuli-responsiveness of nanomaterials to enable local and/or targeted delivery to reduce the treatment side effects.Indeed,the physicochemical versatility of nanomaterials affords many degrees of freedom that enable rational design of smart or autonomous therapeutics,which cannot be achieved using conventional antibiotics.The design straddles the fields of catalysis,nanoscience,microbiology,and translational medicine.To provide an overview of this interdisciplinary landscape,this review is organized based on composition into lipid,metal,metal oxide,and non-metallic nanomaterials.Liposomes as a delivery vehicle enhance bioavailability and reduce toxicity.Metal-and metal oxide-based nanomaterials inhibit bacterial growth by mimicking natural enzymatic activities such as peroxidase(POD)and oxidase.Furthermore,carbon-,polymer-,and cell membrane-based nanomaterials are combined into a discussion on non-metallic materials.At the end of this review,potentially fruitful directions for future bioinspired nanomaterials in infectious disease treatment are included.

关键词： bioinspired nanomaterial bacteria infectious disease antimicrobial liposome nanozyme

Geometric and defects engineering collaboration for enhanced cascade enzymatic nanoreactors

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Nano Research 2024年第4期17卷 2451-2461页

作者： Zhichao Yu Ruijin Zeng Hexiang Gong Yuan Gao Shuyun Chen Yunsen Wang Dianping Tang Key Laboratory for Analytical Science of Food Safety and Biology(MOE&Fujian Province) Department of ChemistryFuzhou UniversityFuzhou 350108China

Highly evolved multi-enzyme cascade catalytic reactions in organisms facilitate rapid transfer of substrates and efficient conversion of intermediates in the catalytic unit,thus rationalizing their efficient biocatalysis.In this study,pore-ordered mesoporous single-atom(Fe)nitrogen-doped carbon nanoreactors(Mp-Fe-CN)were designed,in which a reasonable pore size was designed as a natural enzyme trap coupled to a simulated enzyme center.A polarity-mediated strategy was developed to obtain atomically dispersed nanoporous substrates,with the finding that polarity-guided engineering of the nitrogen-ligand environment and vacancy cluster defects clearly affects nanoporous activity,accompanied by appreciable mesoporous pore size elevation.The active center and distal N atom coordination of Fe-N_(4) affect the catalytic process of the nanozyme exposed by density functional theory(DFT),determining the contribution of hybridized orbitals to electron transfer and the decisive step.A cascade nanoreactor-based domain-limited sarcosine oxidase developed for non-invasive monitoring of sarcosine levels in urine for evaluation of potential prostate carcinogenesis as a proof of concept.Based on the design of surface mesoporous channels of nanocatalytic units,a bridge was built for the interaction between nanozymes and natural enzymes to achieve cascade nanocatalysis of natural enzymatic products.

关键词： nanozyme single-atom catalyst bioreactor cascade catalysis non-Invasive sensing

Copper-based nanomaterials as peroxidase candidates for intelligent colorimetric detection and antibacterial applications

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Particuology 2024年第1期84卷 126-135页

作者： Yanyan Huang Huimin Zhong Cong Jiang Jiahui Yang Jingwen Zhang Fei Zhao Chaoqun Liu College of Light Industry and Food Engineering Nanjing Forestry UniversityNanjing210037China College of Pharmacy Institutes of Environment and MedicineHenan UniversityKaifeng475004China

With natural polyphenol compound tannic acid(TA)as the ingredient,copper tannate(CuTA)nanolayer material was formed by self-assembly under the conditions of heating and copper ion.Copper ion and tannic acid could coordinate to form Cu-O-C structure which was similar to the Fe-N-C structure of natural heme enzymes.In addition,the obtained CuTA nanomaterial possessed excellent peroxidase-like catalytic activity and stability.Based on this excellent enzymatic activity,CuTA nanomaterials could be used for colorimetric detection of hydrogen peroxide with a smartphone and decomposition of organic dyes.Based on the structural characteristics and catalytic activity,the copper tannate nanozymes could also serve as potential antibacterial reagents to effectively inhibit the growth of gram-negative and positive bacteria in a low hydrogen peroxide level.This work may promote the exploration of novel peroxidase mimetics and broaden the applications of nanozymes.

关键词： nanozyme Colorimetric detection Smartphone Antibacteria

Graphdiyne oxide substrate-enhanced peroxidase-mimicking performance of Ru nanoparticles with physiological pH preference

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Nano Research 2024年第3期17卷 1123-1131页

作者： Cong Xu Wenjie Ma Haozhi Wang Leihou Shao Weiqi Li Ping Yu Lanqun Mao Beijing National Laboratory for Molecular Science Key Laboratory of Analytical Chemistry for Living BiosystemsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China State Key Laboratory of Marine Resource Utilization in South China Sea School of Materials Science and EngineeringHainan UniversityHaikou 570228China College of Chemistry Beijing Normal UniversityBeijing 100875China

Modulating electronic structure of metal nanoparticles via metal–support interaction has attracted intense interest in the field of catalytic science.However,the roles of supporting substrates in regulating catalytic properties of nanozymes remain elusive.In this study,we find that the use of graphdiyne oxide(GDYO)as the substrate for self-terminating growth of Ru nanoparticles(Ru@GDYO)endows the peroxidase-like activity of Ru nanoparticles with intrinsic physiological pH preference and natural horseradish peroxidase(HRP)comparable performance.Ru nanoparticles electrolessly deposited onto GDYO possess a partially oxidized electronic structure owing to limited charge transfer between Ru and GDYO,contributing to the intrinsic physiological pH preference of the peroxidase-mimicking nanozyme.More importantly,the substrate GDYO plays an influential factor in enhancing catalytic activity,that is,the activity of Ru@GDYO is much higher than that of Ru nanoparticles deposited on other carbon substrates including graphene oxides and graphdiyne.To demonstrate the application of Ru@GDYO nanozyme in neutral solutions,we employ Ru@GDYO with nicotinamide adenine dinucleotide(NAD+)-dependent dehydrogenases in physiological conditions to realize a sustainable cascade reaction by means of forming continuous NAD^(+)/dihydronicotiamide adenine dinucleotide(NADH)recycling.Our finding represents a promising perspective on designing high-performance peroxidase-mimicking nanozymes with broader applicability,raising fundamental understanding of structure–activity relationship,and investigating new applications of nanozymes in biological systems.

关键词： nanozyme graphdiyne reactive oxygen species electroless deposition metal–support interaction

A functional hydrogenase mimic that catalyzes robust H_(2) evolution spontaneously in aqueous environment

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Nano Research 2024年第5期17卷 3942-3949页

作者： Ningning Song Zhanjun Guo Shuo Wang Yongli Li Yunpeng Liu Meishuai Zou Minmin Liang Experimental Center of Advanced Materials School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China School of Materials Science&Engineering Beijing Institute of TechnologyBeijing 100081China Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China

Although great progress has been made in improving hydrogen production,highly efficient catalysts,which are able to produce hydrogen in a fast and steady way at ambient temperature and pressure,are still in large demand.Here,we report a[NiCo]-based hydrogenase mimic,NiCo_(2)O_(4) nanozyme,that can catalyze robust hydrogen evolution spontaneously in water without external energy input at room temperature.This hydrogenase nanozyme facilitates water splitting reaction by forming a three-center Ni-OH-Co bond analogous to the[NiFe]-hydrogenase reaction by using aluminum as electron donor,and realizes hydrogen evolution with a high production rate of 915 L·h^(-1) per gram of nanozymes,which is hundreds of times higher than most of the natural hydrogenase or hydrogenase mimics.Furthermore,the NiCo_(2)O_(4) nanozyme can robustly disrupt the adhesive oxidized layer of aluminum and enable the full consumption of electrons from aluminum.In contrast to the often-expensive synthetic catalysts that rely on rare elements and consume high energy,we envision that this NiCo_(2)O_(4) nanozyme can potentially provide an upgrade for current hydrogen evolution,accelerate the development of scale-up hydrogen production,and generate a clean energy future.

关键词： hydrogenase mimic nanozyme hydrogen evolution reaction aluminum activation water-splitting

Highly exposed Cu active sites as efficient peroxidase mimics for colorimetric analysis

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ChemPhysMater

ChemPhysMater 2024年第2期3卷 204-211页

作者： Hengya Wei Shushu Chu Fangning Liu Shengzhen Li Yizhong Lu School of Materials Science and Engineering University of JinanJinan 250022China

nanozymes are nanomaterials with intrinsic enzyme-mimic activity,but their large-scale application is generally limited by their low catalytic activity.Herein,we demonstrated that highly exposed Cu active sites on two-dimensional(2D)nitrogen-doped carbon(Cu_(x)/NC)can serve as efficient peroxidase-like(POD)catalysts with high atomic utilization.Specially,the uniformly distributed Cu active sites could react with H_(2)O_(2)to produce singlet oxygen(^(1)O_(2))under acidic conditions,which can efficiently oxidizes colorless 3,3',5,5'-tetramethylbenzidine(TMB)to blue oxidized TMB(oxTMB).Among various Cu_(x)/NC nanozymes studied,the Cuo.14/NC exhibited smaller maximum catalytic velocities(V_(max))and Menten constant(K_(m))for TMB and H_(2)O_(2).Benefiting from the highly active peroxidase-like activity,the Cu_(0.14)/NC nanozyme could be successfully applied for the hydroquinone(HQ)and ascorbic acid(AA)detection applications through the inhibitory effect of HQ and AA.More interestingly,α-glucosidase(α-Glu)detection sensing platform could be constructed based on HQ as a signal transmitter,with the detection range ranging from O to 12 U/L and the minimum detection limit being 0.68 U/L.This work provides not only an idea for the rational design of highly exposed Cu active sites but also fabricate an effective detection sensing platform forHQ,AA,andα-Glu detection.

关键词： nanozyme Highly exposed active sites Peroxidase-like α-glucosidase Sensing

nanozyme:A promising tool from clinical diagnosis and environmental monitoring to wastewater treatment

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Particuology 2022年第12期71卷 90-107页

作者： Chaoyi Hong Xiangqin Meng Jiuyang He Kelong Fan Xiyun Yan CAS Engineering Laboratory for nanozyme Key Laboratory of Protein and Peptide PharmaceuticalInstitute of BiophysicsChinese Academy of SciencesBeijing 100101China School of Future Technology University of Chinese Academy of SciencesBeijing 101408China nanozyme Medical Center School of Basic Medical SciencesZhengzhou UniversityZhengzhou 450052China

Natural enzymes,owing to their outstanding catalytic efficiency and substrate specificity,have been used in a variety of applications including clinical diagnosis,environmental monitoring and wastewater treatment.However,they face inevitable problems such as relatively high cost and lack of stability,dramatically hindering their practical applications in the industry.Recently,a class of nanomaterial that possesses intrinsic enzyme-like properties,nanozyme,has emerged exhibiting numerous advantages over its natural counterpart and has been used as a viable enzyme alternative.In the past decade there are many reviews on nanozyme.The previous discussions tend to view nanozyme as a type of nanomaterial rather than an enzyme.However,it is the enzyme-like activity of nanozymes that provides foundation for their application and nanozymes with the same enzymatic activity usually have some regularity in application.Herein,in this review,we attempt to classify nanozymes by their enzyme-like activity to explain the application principle and relevant cases of nanozymes in clinical diagnosis,environmental monitoring and wastewater treatment,expecting to promote deeper thinking of nanozymes as enzyme mimics and provide useful guidance for future research.

关键词： nanozyme Enzymatic activity Clinical diagnosis Environmental monitoring Wastewater treatment