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Silicon dioxide-protection boosting the peroxidase-like activity of Fe single-atom catalyst for combining chemo-photothermal therapy

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Nano Research 2024年第6期17卷 4924-4933页

作者： Yu Fan Yu Yi Hongpan Rong Jiatao Zhang Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China CAS Center for Excellence in Nanoscience CAS KeyLaboratory for Biomedical Effects of Nanomaterials and NanosafetyNational Center for Nanoscience and Technology(NCNST)Beijing 100190China Key Laboratory of Medical Molecule Science and Pharmaceutics Engineering Ministry of Industry and Information TechnologySchool of Chemistry&Chemical EngineeringBeijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green ApplicationsSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China

Carbon-based single-atom catalysts(SACs)have been widely studied in the field of biomedicine due to their excellent catalytic performance.However,carbon-based SACs usually aggregate during pyrolysis,which leads to the reduction of catalytic activity.Here,we describe a method to improve the monodispersion of SACs using silicon dioxide as a protective layer.The decoration of silicon dioxide serves as a buffer layer for individual nanoparticles,which is not destroyed during the pyrolysis process,ensuring the single-particle dispersion of the nanoparticles after etching.This approach increased the hydroxyl groups on the surface of Fe-SAC(Fe-SAC-SE)and improved its water solubility,resulting in a four times enhancement of the peroxidase(POD)-like activity of Fe-SAC-SE(58.4 U/mg)than that of non-protected SACs(13.9 U/mg).The SiO_(2)-protection approach could also improve the catalytic activities of SACs with other metals such as Mn,Co,Ni,and Cu,indicating its generality for SACs preparation.Taking advantage of the high POD-like activity,photothermal properties,and large specific surface area of Fe-SAC-SE,we constructed a synergistic therapeutic system(Fe-SAC-SE@DOX@PEG)for combining the photothermal therapy,catalytic therapy,and chemotherapy.It was verified that the photothermal properties of Fe-SAC-SE@DOX@PEG could effectively improve its POD-like activity,exhibiting excellent tumor-killing performance at the cellular level.This work may provide a general approach to improve the performances of SACs for disease therapy and diagnosis.

关键词： single-atom catalysts peroxidase-like activity SiO2-protection photothermal therapy catalytic therapy chemotherapy

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Biocompatible carbon nitride quantum dots nanozymes with high nitrogen vacancies enhance peroxidase-like activity for broadspectrum antibacterial

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Nano Research 2023年第5期16卷 7237-7247页

作者： Xiaohui Dai Huan Liu Wenxiao Du Jie Su Lingshuai Kong Shouqing Ni Jinhua Zhan Key Laboratory of Colloid and Interface Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringState Key Laboratory of Crystal MaterialsShandong UniversityJinan 250100China School of Environmental Science and Engineering Shandong UniversityJinan 250100China Institute of Eco-Environmental Forensics Shandong UniversityQingdao 266237China

Nanozyme antibacterial agents with high enzyme-like catalytic activity and strong bacteria-binding ability have provided an alternative method to efficiently disinfect drug-resistance microorganism.Herein,the carbon nitride quantum dots(CNQDs)nanozymes with high nitrogen vacancies(NVs)were mass-productively prepared by a simple ultrasonic-crushing method assisted by propylene glycol.It was found that the NVs of CNQDs were stemmed from the selective breaking of surface N-(C)_(2)sites,accounting for 6.2%.Experiments and density functional theory(DFT)simulations have demonstrated that the presence of NVs can alter the local electron distribution and extend theπ-electron delocalization to enhance the peroxidase-like activity.Biocompatible CNQDs could enter inside microorganisms by diffusion and elevate the bacteria-binding ability,which enhanced the accurate and rapid attack of·OH to the microorganisms.The sterilization rate of CNQDs against Gram-negative bacteria(E.coli),Gram-positive bacteria(S.aureus,B.subtilis),fungi(R.solani)reaches more than 99%.Thus,this work showed great potential for engineered nanozymes for broad-spectrum antibacterial in biomedicine and environmental protection.

关键词： carbon nitride quantum dots(CNQDs) nitrogen vacancies(NVs) peroxidase-like activity biocompatible broad-spectrum antibacterial

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Green synthesis of Au@WSe_(2) hybrid nanostructures with the enhanced peroxidase-like activity for sensitive colorimetric detection of glucose

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Nano Research 2022年第2期15卷 1587-1592页

作者： Chengyi Hong Lingling Chen Chenyue Wu Dan Yang Jia-Yong Dai Zhiyong Huang Ren Cai Weihong Tan College of Food and Biological Engineering Fujian Provincial Key Laboratory of Food Microbiology and Enzyme EngineeringJimei UniversityXiamen 361021China Molecular Science and Biomedicine Laboratory State Key Laboratory for Chemo/Bio-Sensing and ChemometricsCollege of Chemistry and Chemical EngineeringCollege of Biology College of Material Science and Engineeringand Collaborative Research Center of Molecular Engineering for TheranosticsHunan UniversityChangsha 410082China RMIT University MelbourneVIC 3000Australia Key Laboratory of Musculoskeletal System Degeneration and Regeneration Translational Research of Zhejiang Province Sir Run Run Shaw HospitalMedical College of Zhejiang UniversityHangzhou 310016China

We report a colorimetric method for glucose detection based on Au nanoparticle-decorated WSe_(2)(Au@WSe_(2))hybrid nanostructures.These hybrid structures are easily synthesized by simply stirring HAuCl_(4) precursor with WSe_(2) nanosheets in aqueous solution.Owing to strong synergistic catalytic effects of Au nanoparticles and WSe_(2) nanosheets,the Au@WSe_(2) hybrid nanostructures exhibit enhanced peroxidase-like activity(about 2-fold higher compared to WSe_(2) nanosheets alone)for 3,3',5,5'-tetramethylbenzidine oxidation by H_(2)O_(2).Based on the highly catalytical property,the colorimetric method for glucose detection is established by coupling glucose oxidase(GOx).The detection limit of glucose is 3.66 pM.Moreover,the proposed colorimetric method is applicable to glucose detection in serum samples and is promising for applications in biomedical fields.

关键词： Hybrid nanomaterials peroxidase-like activity two-dimensional nanomaterials glucose detection

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Palladium Nanoparticles/Graphdiyne Oxide Nanocomposite with Excellent peroxidase-like activity and Its Application for Glutathione Detection

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Chemical Research in Chinese Universities 2022年第2期38卷 529-534页

作者： LAN Weifei HU Ruifeng HUANG Danrong DONG Xu SHEN Gangyi CHANG Shan DAI Dongsheng School of Pharmacy Minzu University of ChinaBeijing 100081P.R.China Institute of Chemistry Chinese Academy of SciencesBeijing 100190P.R.China Institute of Bioinformatics and Medical Engineering School of Electrical and Information EngineeringJiangsu University of TechnologyChangzhou 213001P.R.China

In this study, palladium nanoparticles loaded graphdiyne oxide (Pd/GDYO) nanocomposite were fabricated by in-situ reduction of palladium chloride in the dispersion of GDYO, and characte-rized by Raman spectra, transmission electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy. The synthesized Pd/GDYO was first found to have catalytic activities similar to those of the peroxidase enzyme, which can catalyze the oxidation of peroxidase substrate 3,3',5,5'-tetramethylbenzidine(TMB) in the presence of hydrogen peroxide(H2O2). Steady-state kinetic studies showed that the catalytic reaction of Pd/GDYO follows a ping-pong mechanism, and Pd/GDYO has a stronger activity to TMB with a Michaelis constant(Km) value of 5.32×10-4 mmol/L. Based on the shielding effect of glutathione(GSH) on the Pd/GDYO-H2O2-TMB reaction system, a colorimetric detection method for GSH was deve-loped with a wide linear range from 0.1 μmol/L to 40 μmol/L and a limit of detection of 0.1 μmol/L. The method was successfully applied for fast and accurate detection of GSH in injection powder drugs. It was expected that this peroxidase-like Pd/GDYO nano- composite would have wide applications in the fields of biomedicine and environmental chemistry.

关键词： Palladium nanoparticle/graphdiyne oxide nanocomposite peroxidase-like activity Colorimetric detection Glutathione

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One-pot synthesis of bimetallic Fe/Co incorporated silica hollow spheres with superior peroxidase-like activity

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Chinese Chemical Letters 2023年第7期34卷 414-417页

作者： Wenli Zhao Wenhao Wang Fancang Meng Yang Du Qingmin Ji Heng-Dao Quan Herbert Gleiter Institute for Nanoscience School of Materials Science and EngineeringNanjing University of Science&TechnologyNanjing 210094China School of Chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China School of Chemistry and Chemical Engineering Beijing Institute of TechnologyBeijing 100081China

Mesoporous silica hollow spheres with a homogenous and high content distribution of Fe and Co were synthesized by a facile one-pot hydrothermal process. The sub-nanometer bimetallic components inside the silica framework facilitate the stable fixation and the open accessibility to active sites. The co-doped Fe/Co in the spheres showed excellent peroxidase-like activity and much higher catalytic performance than their monometallic-supported spheres. The synergistic effect between Fe and Co promotes the continuous formation of functional radicals during the oxidation process and thus accelerates the reaction rate. When used for colorimetric detection of hydrogen peroxide(H_(2)O_(2)), the Fe/Co incorporated silica hollow spheres show the capability of detection of H_(2)O_(2) in a wide range(10-250 μmol/L) and with the low detection limit of 0.012 ppm.

关键词： Bimetallic doping Mesoporous silica Hollow sphere Supported catalyst peroxidase-like activity

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Highly sensitive nanozyme strip:An effective tool for forensic material evidence identification

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Nano Research 2024年第3期17卷 1785-1791页

作者： Juanji Hong Zhanjun Guo Dihan Duan Yi Zhang Xin Chen Yongjiu Li Zheng Tu Lei Feng Lei Chen Xiyun Yan Lizeng Gao Minmin Liang Demin Duan Experimental Center of Advanced Materials School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China College of Bioscience and Biotechnology Shenyang Agricultural UniversityShenyang 110866China Chongqing kangjuquanhong biology science and technology Co. ltdChongqing 400026China Key Laboratory of Forensic Genetics Institute of Forensic ScienceMinistry of Public SecurityBeijing 100038China CAS Engineering Laboratory for Nanozyme Key Laboratory of BiomacromoleculesInstitute of BiophysicsChinese Academic of ScienceBeijing 100101China

During criminal case investigations,blood evidence tracing is critical for criminal investigation.However,the blood stains are often cleaned or covered up after the crime,resulting in trace residue and difficult tracking.Therefore,a highly sensitive and specific method for the rapid detection of human blood stains remains urgent.To solve this problem,we established a nanozyme-based strip for rapid detection of blood evidence with high sensitivity and specificity.To construct reliable nanozyme strips,we synthesized CoFe_(2)O_(4) nanozymes with high peroxidase-like activity by scaling up to gram level,which can be supplied for six million tests,and conjugated antibody as a detection probe in nanozyme strip.The developed CoFe_(2)O_(4) nanozyme strip can detect human hemoglobin(HGB)at a concentration as low as 1 ng/mL,which is 100 times lower than the commercially available colloidal gold strips(100 ng/mL).Moreover,this CoFe_(2)O_(4) nanozyme strip showed high generality on 12 substrates and high specificity to human HGB among 13 animal blood samples.Finally,we applied the developed CoFe_(2)O_(4) nanozyme strip to successfully detect blood stains in three real cases,where the current commercial colloidal gold strip failed to do.The results suggest that the CoFe_(2)O_(4) nanozyme strip can be used as an effective on-scene detection method for human blood stains,and can further be used as a long-term preserved material evidence for traceability inquiry.

关键词： CoFe_(2)O_(4)nanozyme nanozyme strip peroxidase-like activity human hemoglobin blood evidence

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Tuning Atomically Dispersed Fe Sites in Metal–Organic Frameworks Boosts peroxidase‑like activity for Sensitive Biosensing

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Nano-Micro Letters 2020年第12期12卷 392-403页

作者： Weiqing Xu Yikun Kang Lei Jiao Yu Wu Hongye Yan Jinli Li Wenling Gu Weiyu Song Chengzhou Zhu Key Laboratory of Pesticide and Chemical Biology of Ministry of Education International Joint Research Center for Intelligent Biosensing Technology and HealthCollege of ChemistryCentral China Normal UniversityWuhan 430079People’s Republic of China State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing 102249People’s Republic of China

Although nanozymes have been widely developed,accurate design of highly active sites at the atomic level to mimic the electronic and geometrical structure of enzymes and the exploration of underlying mechanisms still face significant challenges.Herein,two functional groups with opposite electron modulation abilities(nitro and amino)were introduced into the metal–organic frameworks(MIL-101(Fe))to tune the atomically dispersed metal sites and thus regulate the enzymelike activity.Notably,the functionalization of nitro can enhance the peroxidase(POD)-like activity of MIL-101(Fe),while the amino is poles apart.Theoretical calculations demonstrate that the introduction of nitro can not only regulate the geometry of adsorbed intermediates but also improve the electronic structure of metal active sites.Benefiting from both geometric and electronic effects,the nitro-functionalized MIL-101(Fe)with a low reaction energy barrier for the HO*formation exhibits a superior POD-like activity.As a concept of the application,a nitro-functionalized MIL-101(Fe)-based biosensor was elaborately applied for the sensitive detection of acetylcholinesterase activity in the range of 0.2–50 mU mL−1 with a limit of detection of 0.14 mU mL−1.Moreover,the detection of organophosphorus pesticides was also achieved.This work not only opens up new prospects for the rational design of highly active nanozymes at the atomic scale but also enhances the performance of nanozyme-based biosensors.

关键词： Nanozymes Metal–organic frameworks Atomically dispersed sites peroxidase-like activity Biosensors

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Large scale and controllable preparation of W2C nanorods or WC nanodots with peroxidase-like catalytic activity

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Chinese Physics B 2017年第4期26卷 484-488页

作者：任晓娜夏敏燕青芝葛昌纯 Institute of Nuclear Energy and New Energy System Materials School of Materials Sciences and EngineeringUniversity of Science and Technology Beijing(USTB)Beijing 100083China

WC nanorods or WC nanodots are prepared via an easy,shape-controllable and large-scale preparation technique.Results reveal that each of the WC nanorods and WC nanodots has a peroxidase-like activity.Besides,the peroxidase-like activity of WC is the first time to be demonstrated.The catalytic efficiency of WC nanorods is much higher than that of WC nanodots and chemical condition range of WC can be wider than that of WC,which indicates that WC is likely to be used as artificial mimetic peroxidase or in-situ amplified colorimetric immunoassay.

关键词： W2C nanorods WC nanodots peroxidase-like activity mesoporous carbon

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Single-layer Rh nanosheets with ultrahigh peroxidase-like activity for colorimetric biosensing

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Nano Research 2018年第12期11卷 6304-6315页

作者： Shuangfei Cai Wei Xiao Haohong Duan Xixi Liang Chen Wang Rong Yang Yadong Li CAS Key Lab for Biomedical Effects of Nanomaterials and Nanosafety CAS Center for Excellence in NanosdenceNational Center for Nanoscience and TechnologyUniversity of Chinese Academy of SciencesBeijing 100190China Chemistry Research Laboratory Department of ChemistryUniversity of Oxford12 Mansfield RoadOxford OX13TAUK Department of Chemistry Tsinghua UniversityBeijing 100084China

When the dimensionality of layered compounds decreases to the physical limit, ultimate two-dimensional (2D) anisotropy and/or quantum confinement effects may lead to extraordinary physicochemical attributes. Here, we report single-layer Rh nanosheets (NSs) exhibiting ultrahigh peroxidase-like activity, far exceeding that of horseradish peroxidase (HRP) and of most known layered nanomaterial-based peroxidase mimics. Considering per NS as an active subunit, the Rh NSs displayed a catalytic rate constant (Kcat) as high as 4.45 × 105 s–1 to H2O2, two orders of magnitude higher than those of HRP and Rh nanoparticles. The high atom efficiency of the Rh NSs can be attributed to the full exposure of surface-active Rh atoms, which greatly facilitates electron transfer and formation of superoxide anions, representing reactive oxygen species in the catalytic process. As a proof-of-concept application, the Rh NSs were successfully used as peroxidase mimics for the colorimetric detection of H2O2 and xanthine, with high sensitivity and selectivity. Moreover, a simple, rapid, and sensitive Rh-based paper sensor for ascorbic acid was also developed. In summary, this work provides a novel example of single-layer metallic NSs for biosensing.

关键词： Rh nanosheets nanozymes peroxidase-like activity colorimetric detection

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Incorporation of Fluorescent Carbon Quantum Dots into Metal-Organic Frameworks with peroxidase-Mimicking activity for High-Performance Ratiometric Fluorescent Biosensing

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Journal of Analysis and Testing 2023年第1期7卷 16-24页

作者： Qiuyu Ye Tao Dai Jin Shen Qin Xu Xiaoya Hu Yun Shu School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China

A new ratiometric fluorescent sensor based on the bifunctional carbon quantum dots(CQDs)@metal-organic framework(MOF)nanocomposite possessing peroxidase-mimicking catalytic and luminescent characteristics was developed for hydrogen peroxide(H_(2)O_(2))and cholesterol detection.The incorporation of fluorescent CQDs into the cavities of MIL-101(Fe)MOF with peroxidase-like activities endows the nanocomposite with bifunctional properties.The CQDs@MOF can oxidize o-phenylene-diamine to 2,3-diaminophenolazine by H_(2)O_(2)with yellow fluorescence(556 nm).Meantime,the intrinsic fluorescence signal(455 nm)of CQDs@MOF is inhibited due to the inner filter effect.Therefore,the ratio of the fluorescent intensity is employed as the signal output to construct the H_(2)O_(2)ratiometric biosensor.In addition,the cholesterol can be determined by the ratiometric sensor with high sensitivity.In addition,the total cholesterol in human serum is determined with high accuracy using our ratiometric biosensor.This ratiometric fluorescent platform based on the bifunctional CQDs@MOF provides new insights in the field of bio-sensing.

关键词： Carbon quantum dots Metal-organic framework peroxidase-like activity Ratiometric fluorescent detection

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