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Diatomic active sites nanozymes:Enhanced peroxidase-like activity for dopamine and intracellular H2O2 detection

Nano Research 2022年第5期15卷 4266-4273页

作者： Shan Wang Zunfu Hu Qiulian Wei Huimin Zhang Weina Tang Yunqiang Sun Haiqiang Duan Zhichao Dai Qingyun Liu Xiuwen Zheng Key Laboratory of Functional Nanomaterials and Technology in Universities of Shandong College of Chemistry and Chemical EngineeringLinyi UniversityLinyi 276000China School of Chemical and Biological Engineering Shandong University of Science and TechnologyQingdao 266510China School of Materials Science and Engineering Linyi UniversityLinyi 276000China

Considering intracellular hydrogen peroxide(H_(2)O_(2))plays pivotal roles in the regulation of serial biological processes,the in-situ detection of intracellular H2O2 has attracted an extensive attention.In the present work,an atomically dispersed diatomic active sites Nanozymes(FeN_(3)/PtN_(4)-single-atom nanozymes(SAzyme))was prepared exhibiting enhanced peroxidase-like activity.The obvious synergistic effect between Fe-Pt heteronuclear diatomic active sites was confirmed by series of characterization and density functional theory(DFT).The peroxidase-like activity of Fe-sites could be substantially enhanced by the bonded Pt-sites via the modulation effect.As a consequence,the gap between the d-band centre(εd)of Fe 3d orbitals and the Fermi energy level was narrowed and the electronic interaction could be strengthened,leading to a lower free energy barrier and a lower activation energy as well as fortified metal-O bonding in the kinetic pathway.Therefore,the constructed FeN3/PtN4-SAzyme exhibited higher peroxidase-like activity than that of FeN4-SAzyme.The FeN3/PtN4-SAzyme-assisted oxidation of 3,3',5,5'-tetramethylbenzidine(TMB)facilitated the colorimetric detection of dopamine(DA),an important biomolecule.The linear detection range and limit of detection(LOD)of DA and H_(2)O_(2) were 1-10 μM,0.01-1.0 mM and 0.109 μM,7.97 μM,respectively.In addition,the constructed SAzymes were also applied for the in-situ detection of intracellular H2O2,expanding the application scope of the newborn SAzymes.

关键词： single-atom nanozymes heteronuclear diatomic active sites peroxidase-like dopamine intracellular H_(2)O_(2)

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Synergistic Lewis acid-base sites of ultrathin porous Co_(3)O_(4)nanosheets with enhanced peroxidase-like activity

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Nano Research 2021年第10期14卷 3514-3522页

作者： Wenhui Lu Ming Yuan Jing Chen Jiaxin Zhang Lingshuai Kong Zhenyu Feng Xicheng Ma Jie Su Jinhua Zhan Key Laboratory of Colloid and Interface Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringState Key Laboratory of Crystal MaterialsShandong UniversityJinan 250100China

Surface Lewis acid-base sites in crystal structure may influence the physicochemical properties and the catalytic performances in nanozymes.Understanding the synergistic effect mechanism of Co_(3)O_(4)nanozymes towards substances(3,3’,5,5’-tetramethylbenzidine(TMB)and hydrogen peroxide(H2O2))induced by surface Lewis acid-base sites is important to enhance the efficiency for peroxidase-like reaction.Herein,ultrathin porous Co_(3)O_(4)nanosheets with abundant Lewis acid-base sites were prepared by sodium borohydride(NaBH4)reduction treatment,which exhibited high-efficiency peroxidase-like activity compared with original Co_(3)O_(4)nanosheets.The Lewis acid-base sites for ultrathin porous Co_(3)O_(4)nanosheets nanozyme were owing to the coordination unsaturation of Co ions and the formation of defect structure.Ultrathin porous Co_(3)O_(4)nanosheets had 18.26-fold higher catalytic efficiency(1.27×10^(-2)s^(-1)·mM^(-1))than that of original Co_(3)O_(4)(6.95×10^(-4)s^(-1)·mM^(-1))in oxidizing TMB substrate.The synergistic effect of surface acid and base sites can enhance the interfacial electron transfer process of Co_(3)O_(4)nanosheets,which can be a favor of absorption substrates and the generation of reactive intermediates such as radicals.Furthermore,the limit of detection of hydroquinol was 0.58μM for ultrathin porous Co_(3)O_(4)nanosheets,965-fold lower than original Co_(3)O_(4)(560μM).Besides,the linear range of ultrathin porous Co_(3)O_(4)nanosheets was widely with the concentration of 5.0-1,000μM.Colorimetric detection of hydroquinol by agarose-based hydrogel membrane was provided based on excellent peroxidase-like properties.This study provided insights into designing high-performance nanozymes for peroxidase-like catalysis via a strategy of solid surface acid-base sites engineering.

关键词： cobalt oxide nanozyme Lewis acid-base sites peroxidase-like colorimetric sensor hydroquinol

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Synergistic Effect of Sandwich Polyoxometalate and Copper-Imidazole Complexe for Enhancing peroxidase-like Activity

Synergistic Effect of Sandwich Polyoxometalate and Copper-Im...

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中国化学会第九届全国无机化学学术会议

作者： Dong-Feng Chai Yun-Feng Qiu Hong Liu Department of Chemistry College of Pharmacy Jiamusi University State Key Laboratory of Robotics and System (HIT) Academy of Fundamental and Interdisciplinary SciencesHarbin Institute of Technology

H2O2 detection has attracted much attention in recent years due to that its production may affect many biochemistry reactions in the body that may be dangerous for human health.[1-3] Herein, an inorganic-organic hybrid based on copper（II）-imidazole complexe modified sandwich-type tungstobismuthate, Na4H2[Cu4（H4im）12（H3im）2][Cu3（H2O）6（Bi W9O33）2]·40H2O（H4im = imidazole, H3 im = deprotonated imidazole）（1） has been synthesized and structurally characterized by single crystal X-ray diffraction. Compound 1 was demonstrated to possess high peroxidase-like activity when using 3, 3’, 5, 5’-tetramethylbenzidine（TMB） as a peroxidase substrate in the presence of H2O2. The synergistic effects of sandwich-type polyoxometalate and copper（II）-imidazole complexe is responsible for the enhancement of peroxidase-like activity than polyoxometalate and copper（II）-imidazole complexe. Considering the dependence of TMB coloration on H2O2 concentrations, 1 can be used as an effective biosensor to detect H2O2 through facile colorimetric method in a linear range from 1 μM to 50 μM with a low detection limit of 0.12 μM. Compound 1opens a new approach to the H2O2 sensor by inorganic-organic hybrid compounds.

关键词： Polyoxometalate peroxidase-like enzyme copper-imidazole

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

ChemPhysMater

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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

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Amalgamated gold-nanoalloys with enhanced catalytic activity for the detection of mercury ions(Hg^2+)in seawater samples

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Nano Research 2020年第4期13卷 989-998页

作者： Natasha Logan Claire McVey Christopher Elliott Cuong Cao Institute for Global Food Security School of Biological SciencesQueens University Belfast19 Chlorine GardensBelfastBT95DLUK Material and Advanced Technologies for Healthcare Queens University Belfast18-30 Malone RoadBelfastBT95BNUK

Mercury(Hg)is extremely toxic,and continues to cause major threats to aquatic life,human health and the environment.Hg^2+mainly derives from seawater as a product of atmospheric deposition,therefore there is great demand for sensing approaches that can detect Hg^2+in seawater samples.Herein,we demonstrate that the peroxidase-mimicking activity of gold nanoparticles(AuNPs)or so-called nanozymes,can be exploited for the detection of Hg^2+ions in various water samples.In a high electrolyte environment,the catalytic activity for the oxidation of 3,3’,5,5’-tetramethylbenzidine(TMB)was significantly diminished due to poor stability of the bare-AuNPs.This activity was reduced by-73.7%when the NaCl concentration was higher than 1.168%,which is much lower than that of seawater(-3.5%),thus presenting its unsuitability for detecting Hg^2+in harsh water matrices.To overcome this limitation,AuNPs were first functionalized with oligo-ethylene glycol(OEG),of which their colloidal form presented high stability in NaCl concentrations up to 20%and across a wide range of pHs from 1-14.Interestingly,the catalytic activity of OEG-AuNPs for the oxidation of TMB was strongly suppressed by the coating,but enhanced upon formation of Au-Hg amalgamation.This novel finding underlies a straightforward,sensitive,and highly selective detection platform for Hg^2+in water samples.The approach could detect the exposure limit level for Hg^2+in drinking water(i.e.,2 ppb for tap and bottled water)as set by the United States Environmental Protection Agency(EPA)and the World Health Organization(WHO).When Hg^2+was spiked into a 3.5%saline solution and a coastal seawater certified reference material(CRM),the detection limits were found to be 10 ancM 3 ppb,respectively,which exceed the Hg^2+concentrations commonly found within seawater(-60-80 ppb).The whole procedure takes less than 45 min to conduct,providing a highly innovative,rapid and low-cost approach for detecting Hg^2+in complex water matrices.

关键词： gold nanoparticles nanozyme peroxidase-like mercury detection w ater samples seawater

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Iron oxide nanoparticles with photothermal performance and enhanced nanozyme activity for bacteria-infected wound therapy

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Regenerative Biomaterials 2022年第1期9卷 548-559页

作者： Jiaxin Guo Wenying Wei Yanan Zhao Honglian Dai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Biomedical Materials and Engineering Research Center of Hubei ProvinceWuhan University of TechnologyWuhan 430070China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen ValleyFoshan 528200China Shenzhen Research Institute of Wuhan University of Technology Shenzhen 518000China

Metal-based nanomaterials usually have broad-spectrum antibacterial properties,low biological toxicity and no drug resistance due to their intrinsic enzyme-like catalytic properties and external field(magnetic,thermal,acoustic,optical and electrical)responsiveness.Herein,iron oxide(Fe_(3)O_(4))nanoparticles(IONPs)synthesized by us have good biosafety,excellent photothermal conversion ability and peroxidase-like catalytic activity,which can be used to construct a photothermal-enzymes combined antibacterial treatment platform.IONPs with peroxide-like catalytic activity can induce H_(2)O_(2)to catalyze the production of·OH in a slightly acidic environment,thus achieving certain bactericidal effects and increasing the sensitivity of bacteria to heat.When stimulated by near-infrared light,the photothermal effect could destroy bacterial cell membranes,resulting in cleavage and inactivation of bacterial protein,DNA or RNA.Meanwhile,it can also improve the catalytic activity of peroxidase-like and promote IONPs to catalyze the production of more·OH for killing bacteria.After IONPs synergistic treatment,the antibacterial rate of Escherichia coli and Staphylococcus aureus reached nearly 100%.It also has an obvious killing effect on bacteria in infected wounds of mice and can effectively promote the healing of S.aureusinfected wounds,which has great application potential in clinical anti-infection treatment.

关键词： antibacterial photothermal therapy peroxidase-like catalytic therapy

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Nanocatalytic Medicine of Iron-Based Nanocatalysts

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CCS Chemistry 2021年第2期3卷 2445-2463页

作者： Peilei Liu Minfeng Huo Jianlin Shi State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050 2Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049

Iron can be found in all mammalian cells and is of critical significance to diverse cellular activities within human bodies.Widespread applications and the underlying chemical and biological fundamental explorations of iron-based nanomaterials,especially on the biomedical frontiers,have attracted growing interests most recently in the community.In this review,we focus on the catalytic performance of iron-based nanomaterials(termed as nanocatalysts,abbreviated as NCs)and their nanocatalytic biomedical applications in Fenton nanocatalytic therapeutics,nanocatalytic oxygenation-enabled therapeutics,and nanocatalytic peroxidation-enabled biodetections.Fabrication methodologies of the iron-based NCs are also summarized along with their applications.Representative therapeutic performance against malignant tumors,Alzheimer’s disease(and other pathological abnormalities),and nanocatalyticbased biodetection are discussed.Finally,future development prospects of the iron-based NCs are surveyed,aiming to deliver a brighter future for iron-based NCs in nanocatalytic medicine.

关键词： iron-based nanocatalysts Fenton catalysis,antioxidation peroxidase-like biodetections

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An ultra-highly active nanozyme of Fe,N co-doped ultrathin hollow carbon framework for antibacterial application

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Chinese Chemical Letters 2023年第3期34卷 388-391页

作者： Jinyu Hao Cui Zhang Chenxi Feng Qian Wang Zhong-Yi Liu Yan Li Jianshuai Mu En-Cui Yang Yan Wang College of Chemistry Tianjin Key Laboratory of Structure and Performance for Functional MoleculesTianjin Normal UniversityTianjin 300387China School of Chemistry and Chemical Engineering Harbin Institute of TechnologyHarbin 150001China School of food and Bioengineering Xuzhou University of TechnologyXuzhou 221018China

In recent years, nanozymes have received more and more attention, but the low activity limits the development of nanozymes. Therefore, the design and development of efficient nanozymes is still a major challenge for researchers. Herein, the Fe,N co-doped ultrathin hollow carbon framework(Fe,N-UHCF) exhibit ultra-high peroxidase-like activity. The specific activity of Fe,N-UHCF nanozyme is as high as 36.6 U/mg,which is much higher than almost all of other reported nanozymes. In practical applications, the Fe,N-UHCF show good antibacterial effects.

关键词： peroxidase-like Nanozyme Ultra-highly active Specific activity Antibacterial

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Novel Approach for the Decoration of Magnetic Carbon Nanospheres with Platinum Nanoparticles and Their Enhanced peroxidase Activity for the Colorimetric Detection of H2O2

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Chemical Research in Chinese Universities 2019年第1期35卷 163-170页

作者： SU Ce BAI Lingling ZHANG Hongbo CHANG Kaishan LI Guanbin LI Siliang School of Petrochemical Engineering Lanzhou University of TechnologyLanzhou 730050P.R.China

Pt/Fe3O4-DIB-DETA-CNS(PFDDC)nanocomposite(DIB=2,4-dihydroxybenzaldehyde;DETA=diethylenetfiamine;CNS=carbon nanosphere)was synthesized by dispersing Pt nanoparticles on magnetic carbon nanospheres. The structure,morphology and composition of the nanocomposite were studied by X-ray diffraction(XRD),transmission electron microscopy(TEM),energy-dispersive X-ray spectroscopy(EDX)and X-ray photoelectron spectroscopy(XPS). In addition,the nanocomposite showed superior peroxidase-like activity towards 3,3',5,5'-tetramethylbenzidine(TMB) with a visual color change in the presence of hydrogen peroxide(H2O2).Therefore,the PFDDC nanocomposite provides a sensing platform for the colorimetric detection of H2O2 with high sensitivity and selectivity.Furthermore,the nanocomposite can be conveniently preserved and separated.These features enable the nanocomposite to colorimetrically detect H2O2 for potential pharmaceutical,environmental and industrial applications.

关键词： Pt nanoparticle Magnetic carbon nanosphere peroxidase-like activity Colorimetric sensor H2O2

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