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Hybridization chain reaction-based DNA nanomaterials for biosensing,bioimaging and therapeutics

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Chinese Chemical Letters 2024年第2期35卷 223-231页

作者： Zhaoyue Lv Mengxue Huang Peiran Li Mengdi Xu Chi Yao Dayong Yang Frontiers Science Center for Synthetic Biology Key Laboratory of Systems Bioengineering (MOE)Institute of Biomolecular and Biomedical EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China Zhejiang Institute of Tianjin University Ningbo 315201China

DNA nanomaterials hold great promise in biomedical fields due to its excellent sequence programmability,molecular recognition ability and biocompatibility.Hybridization chain reaction(HCR)is a simple and efficient isothermal enzyme-free amplification strategy of DNA,generating nicked double helices with repeated units.Through the design of HCR hairpins,multiple nanomaterials with desired functions are assembled by DNA,exhibiting great potential in biomedical applications.Herein,the recent progress of HCR-based DNA nanomaterials for biosensing,bioimaging and therapeutics are summarized.Representative works are exemplified to demonstrate how HCR-based DNA nanomaterials are designed and constructed.The challenges and prospects of the development of HCR-based DNA nanomaterials are discussed.We envision that rationally designing HCR-based DNA nanomaterials will facilitate the development of biomedical applications.

关键词： DNA nanotechnology Hybridization chain reaction DNA nanomaterials biosensing Bioimaging Therapeutics

A Label-Free Deoxyribozyme Sensor for m^(6)A Demethylase Activity Detection

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Chinese Journal of Chemistry 2024年第9期42卷 951-956页

作者： Xiuyuan Wang Shusheng Yu Yuqiu He Fuan Wang Xiaoqing Liu College of Chemistry and Molecular Sciences Wuhan UniversityWuhanHubei 430072China

A label-free deoxyribozyme(DNAzyme)biosensor for m^(6) demethylase activity detection is developed.When demethylase FTO(Fat mass and obesity-associated protein),an important m^(6) demethylase of ALKBH demethylase family is present,the m^(6) group is specifically demethylated,and the cleavage activity of DNAzyme is restored.This allows the cleavage product that contains G-quadruplex sequence to bind to thioflavin T(ThT)and generate fluorescence signals.The biosensor shows high specificity and sensitivity,and fast reaction speed.Our study demonstrates a new design of allosteric DNAzyme for sensing.This method represents the first label-free nucleic acid biosensor for FTO assay,providing a feasible route towards inhibitors screening.

关键词： DNAzyme Analytical methods biosensing m^(6)A demethylation Fluorescence

Activity regulation and applications of metal-organic framework-based nanozymes

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Rare Metals 2024年第3期43卷 900-914页

作者： Ge Fang Shou-Xin Bao Gen-Xiu Zhou Cui-Cui Ge State Key Laboratory of Radiation Medicine and Protection School of Radiation Medicine and ProtectionSchool for Radiological and Interdisciplinary Sciences(RAD-X)Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123China Suzhou Nanomicro Technology Co. LtdSuzhou 215000China

As a new generation of artificial enzymes,nanozymes show outstanding advantages such as high stability,low cost,and facile synthesis,which endow them with promising applications in biomedical and environmental fields.Among the various reported nanozymes,metal-organic frameworks(MOFs)could mimic the active center of natural enzymes and provide a hydrophobic environment,which makes MOFs attractive alternatives to natural enzymes.Owing to the highly structural diversity and tailorability of MOFs,rational design will contribute to improve the activity of MOF-based nanozymes and promote their potential applications in both biomedical and environmental fields.Therefore,a comprehensiye suminary of activity regulatory strategies of MOF-based nanozymes is urgently needed.Firstly,we summarized the activity regulatory strategies of MOFs with intrinsic enzyme-like activities via modulation of metal nodes,ligands,structures and morphologies.Then the applications of MOF-based nanozymes in biosensing,hazardous degradation,antibacterial,and cancer therapy were also introduced.Finally,the current challenges and future perspectives were discussed in depth.It is highly expected that this review will provide a better understanding on the rational design of novel high-performance MOF-based nanozymes.

关键词： Metal-organic frameworks(MOF)-based nanozymes Activity regulation biosensing Cancer therapy Hazardous degradation Antibacterial

Real-time and label-free biosensing using moiré pattern generated by bioresponsive hydrogel

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生物活性材料(英文) 2023年第5期23卷 383-393页

作者： Semin Kim Geehong Kim Yong Woo Ji Chae-Eun Moon Yuna Jung Hyung Keun Lee JaeJong Lee Won-Gun Koh Department of Chemical and Biomolecular Engineering Yonsei University50 Yonsei-roSeodaemun-guSeoul120-749Republic of Korea Korea Institute of Machinery&Materials Nano-Convergence Mechanical Systems Research Division156 Gajeongbuk-roYuseong-guDaejeon34103Republic of Korea Department of Ophthalmology Yongin Severance HospitalYonsei University College of Medicine363Dongbaekjukjeon-daeroGiheung-guYongin-siGyeonggi-do16995Republic of Korea Institute of Vision Research Department of OphthalmologyYonsei University College of Medicine50-1 Yonsei-roSeodaemun-guSeoul120-749Republic of Korea Department of Ophthalmology Graduate School of Medical ScienceBrain Korea 21 ProjectYonsei University College of MedicineRepublic of Korea College of Pharmacy Yonsei University85 Songdo Hwawak-roYeonsu-guIncheon26426Republic of Korea Department of Ophthalmology Gangnam Severance HospitalYonsei University College of Medicine211 Eonju-roGangnam-guSeoul06273Republic of Korea Department of Nanomechatronics University of Science and Technology217Gajeong-roYuseong-guDaejeon 34113Republic of Korea

Bioresponsive hydrogels are smart materials that respond to various external stimuli and exhibit great potential as biosensors owing to their capability of real-time and label-free detection.Here,we propose a sensing platform based on bioresponsive hydrogels,employing the concept of moiré patterns.Two sets of line patterns with different pitch sizes are prepared;a hydrogel grating whose pitch size changes according to external stimuli and a reference grating with constant pitch size.The volume changes of the hydrogel caused by external stimuli changes the pitch size of the hydrogel grating,and subsequently,the pitch sizes of the moiré patterns(moiré signal),whose values can be obtained in a real-time and label-free manner through customized moiré microscopy and signal processing.After confirming that the pH-induced swelling of hydrogel could be monitored using moiré patterns,we performed moiré pattern-based detection of specific proteins using protein-responsive hydrogel that underwent shrinking via interaction with target proteins.Brain-derived neurotrophic factor and platelet-derived growth factor were selected as the model proteins,and our proposed system successfully detected both proteins at nanomolar levels.In both cases,the pitch size change of hydrogel grating was monitored much more sensitively using moiré patterns than through direct measurements.The changes in the moiré signals caused by target proteins were detected in ex-vivo environments using a custom-made intraocular lens incorporating the hydrogel grating,demonstrating the capability of the proposed system to detect various markers in intraocular aqueous humor,when implanted in the eye.

关键词： Bioresponsive hydrogel Moirépattern biosensing Intraocular lens Aqueous humor

High-gain signal-on PEDOT:PSS organic photoelectrochemical transistor biosensing modulated by a MXene/MOFs/NiO Schottky heterojunction

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Science China Chemistry 2023年第2期66卷 578-585页

作者： Zheng Li Yi-Tong Xu Jin Hu Ting Wang Fang-Qing Liu Hong Zhou Guang-Xu Chen Peng Lin Wei-Wei Zhao Jing-Juan Xu Hong-Yuan Chen State Key Laboratory of Analytical Chemistry for Life Science School of Chemistry and Chemical EngineeringNanjing UniversityNanjing210023China Shenzhen Key Laboratory of Special Functional Materials&Guangdong Research Center for Interfacial Engineering of Functional Materials College of Materials Science and EngineeringShenzhen UniversityShenzhen518060China Shandong Key Laboratory of Biochemical Analysis College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao266042China School of Environment and Energy State Key Laboratory of Luminescent Materials and DevicesGuangdong Provincial Key Laboratory of Atmospheric Environment and Pollution ControlSouth China University of TechnologyGuangzhou510006China

Herein we report a high-gain signal-on poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)organic electrochemical transistor(OECT)biosensing using an accumulation-mode PEDOT:PSS OECT modulated by a light-fueled MXene/MOFs/Ni O Schottky heterojunction.In such a system,the MXene/MOFs/Ni O Schottky heterojunction exhibited superior gating effect,as it not only enabled the fast-directional charge transfer but also guaranteed the maximal accessibility of the electrolyte to topped 2D MXene with large surface area.In linkage with a bi-enzyme cascade system,the quinone derivatives produced by the cascade reaction of alkaline phosphatase(ALP)and tyrosinase(TYR)could serve as effective electron acceptors for the representative Ti_(3)C_(2)/PCN-224/Ni O heterojunction,underpinning an innovative method for sensitive detection of ALP activity with a low detection limit of 0.001 U L^(-1).Remarkably,the as-developed system demonstrated a remarkable current gain as high as near 10^(4),which to our knowledge is the highest one among existing OECT biosensory devices.This work represents a generic protocol to develop the novel signal-on PEDOT:PSS OECT platform towards biochemical detection and beyond.

关键词： signal-on PEDOT:PSS organic electrochemical transistor biosensing Schottky heterojunction

External stimulation-controlled dynamic DNA devices for biosensing and biomedical applications

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Science China Chemistry 2023年第11期66卷 3105-3115页

作者： Wei Xu Feifei Hu Jiajing Li Jinhua Shang Xiaoqing Liu Yan Zeng Qiong Wu Fuan Wang Department of Gastroenterology Zhongnan Hospital of Wuhan UniversityCollege of Chemistry and Molecular SciencesWuhan UniversityWuhan 430072China School of Medicine Wuhan University of Science and TechnologyWuhan 430081China College of Chemistry and Chemical Engineering Hunan UniversityChangsha 410082China

DNA devices that can recognize molecular inputs and transform them into functional outputs in an autonomous manner have been actively pursued as versatile toolkits for controlled nanofabrication,molecular network regulation,biosensing and cellular function modulation.The introduction of external stimuli-responsive units not only ensures the programmability and functionality of DNA devices themselves,but also confers rapid,remote and reversible dynamic regulation capabilities.This facilitates on-demand activation and expands the application scope of dynamic DNA devices.Herein,an overview of recent advances in the construction of stimuli-responsive DNA devices that respond to different exogenous triggers,including physical stimuli(e.g.,light,thermal,magnetic field,and electric field),chemical stimuli(e.g.,supermolecules,pH,redox,and metal ions),and biological cues(e.g.,protein,biomolecule,and nucleic acid),and their controllable nanofabrication and biomedical application have been provided.The current challenges and potential solutions of these externally responsive DNA devices for their future advancements in this emerging field are also discussed.

关键词： DNA device stimuli-responsiveness on-demand regulation DNAzyme biosensing

Recent Advances in Triplet-Triplet Annihilation Upconversion for Bioimaging and biosensing

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Journal of Analysis and Testing 2023年第4期7卷 327-344页

作者： Wenyue Lin Jiayao Li Hongjuan Feng Fang Qi Ling Huang Tianjin Key Laboratory of biosensing and Molecular Recognition Research Center for Analytical SciencesCollege of ChemistryNankai UniversityTianjin 300071China Frontiers Science Center for New Organic Matter Nankai UniversityTianjin 300071China

Photon upconversion is an anti-Stokes process that converts low-energy photons into high-energy photons.The use of upconversion luminescence can avoid the autofluorescence of biological tissue and realize background-free bioimaging with a high signal-to-noise ratio at a low power density.In addition,the excitation of red or near-infrared light facilitates the reduction of photodamage in biological tissues and subsequent bioimaging of deep tissue features in vivo.Meanwhile,upconversion emission-mediated bio sensing offers both high sensitivity and low detection limits for quantitative analysis of the target substances in complicated biological samples.Due to its high upconversion quantum yield,low excitation power density,and tunable absorption and emission wavelengths,triplet-triplet annihilation upconversion(TTA-UC)has garnered considerable interest for bioimaging and biosensing.This review will introduce the fundamental concepts of TTA-UC,the factors that influence TTA-UC materials,and the methodologies for preparing TTA-UC materials.The important progress of TTA-UC in bioimaging and bio sensing in recent years will also be discussed in detail in vitro and in vivo.Furthermore,the current challenges of TTA-UC in bioimaging and biosensing will be discussed,along with potential solutions.

关键词： Triplet-triplet annihilation upconversion Bioimaging biosensing

Electrochemiluminescence biosensing and bioimaging with nanomaterials as emitters

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Science China Chemistry 2022年第12期65卷 2417-2436页

作者： Yaqiang Feng Ningning Wang Huangxian Ju Research Center of Analytical Instrumentation Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of Ministry of EducationCollege of Chemistry and Materials ScienceNorthwest UniversityXi’an 710127China State Key Laboratory of Analytical Chemistry for Life Science School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China School of Pharmacy Shandong Technology Innovation Center of Molecular Targeting and Intelligent Diagnosis and TreatmentBinzhou Medical UniversityYantai 264003China

The continuous emergence of novel luminophores has been leading the development of electrochemiluminescence(ECL)analysis since the ECL phenomenon of silicon nanoparticles was first reported in 2002.Nanomaterial-based luminophores termed as nanoemitters exhibit great application potential in ECL bioanalysis.In this review,we systematically summarize the research progress of various types of ECL nanoemitters,such as semiconductor quantum dots(QDs),carbon dots(CDs),polymer dots(Pdots),aggregation-induced emission nanoparticles(AIE dots),and other nanoemitters including luminophoredoped silica nanoparticles,metal-organic frameworks,covalent organic frameworks,and metal nanoclusters.We mainly emphasize the characteristic of these nanoemitters and their applications in ECL biosensing and bioimaging by using them as labels,and highlight some impressive cases in the last five years.Finally,we discuss current challenges in the field of ECL nanoemitters and point out their prospects.

关键词： electrochemiluminescence nanoemitters biosensing bioimaging

Deep-Red to Near-Infrared Carbon Dots in biosensing and Bio-medical Applications

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Chinese Journal of Chemistry 2023年第18期41卷 2354-2370页

作者： Shan Huang Li Yan Xiaojun Chen Jun-Jie Zhu Schoolof Chemistry and Molecular Engineering Nanjing TechUniversityNanjingJiangsu 211816China Schoolof Chemistry and chemical Engineering Nanjing UniversityNanjingJiangsu 210023China

Comprehensive Summary,With the rapid development in the field of biomedical diagnosis and treatment,carbon dots(CDs)with favorable photostability,biocompatibility and high quantum yields for deep-red to near-infrared emission have attracted the attention of a majority of researchers.By enlarging the sp2 domain in the core of CDs,doping them with heteroatoms like nitrogen and sulfur,applying hydrothermal,electrochemical,or microwave-assisted techniques,CDs can be made with the aforementioned photoemission capabilities.In view of these excellent properties,CDs are flourishing in biosensing and biomedical applications,so that a thorough description and discussion of this topic is beneficial to capture the up-to-date progress of CDs in this field,providing suggestions and considerations for readers.

关键词： Carbon dots biosensing Biomedical Biotechnology Cancer therapy Antibacterial