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Covalent stabilization of dna nanostructures on cell membranes for efficient surface receptor-mediated labeling and function regulations

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Science China Chemistry 2022年第11期65卷 2327-2334页

作者： Dandan Chao Xuemei Xu Yanyan Miao Linlin Yang Qianqian Gao Rui Xu Yuan Tian Yumeng Zhao Yuzhen Du Da Han Institute of Molecular Medicine Shanghai Key Laboratory for Nucleic Acid Chemistry and NanomedicineState Key Laboratory of Oncogenes and Related GenesRenji HospitalSchool of MedicineShanghai Jiao Tong UniversityShanghai 200127China Department of Laboratory Medicine Shanghai Jiao Tong University Affiliated Sixth People’s HospitalShanghai 200127China

One major challenge of using dna nanostructures for cellular and in vivo applications is their insufficiently structural integrity that stems from the non-covalent base pairing and stacking in complex cellular and physiological environment. The establishment of covalent bonds in dna nanostructures can link individual strands more stably and therefore should improve the performance of dna nanostructures in different scenarios where structural integrity is required. Here, we developed a convenient and effective method for constructing covalently stabilized dna nanostructures by chemically inserting photo-crosslinker(^(CNV)K) in dna sequences. These covalently linked dna nanostructures were found to be more resistant to external interference, such as low cation concentrations and unspecific displacement on cell membranes. We also demonstrated that our strategy could improve the efficiency of cell surface receptor-mediated labeling and function regulations in living cells, which sheds light on broadening the biomedical applications of dna nanostructures.

关键词： dna nanostructures covalent stabilization structural integrity cell labeling surface receptor regulation

Functionalizing dna nanostructures with natural cationic amino acids

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Bioactive Materials 2021年第9期6卷 2946-2955页

作者： Dong Wang Chunfa Chen Qian Liu Qianwen Zhao Di Wu Yue Yuan Chaowang Huang Xiaorong Sun Chunji Huang David Tai Leong Guansong Wang Hang Qian Institute of Respiratory Diseases Xinqiao HospitalThird Military Medical University183 Xinqiao StreetChongqing400037China Laboratory of Pharmacy and Chemistry And Laboratory of Tissue and Cell BiologyLab Teaching&Management CenterChongqing Medical UniversityChongqing400016China Basic Medical College Third Military Medical UniversityChongqing400038China Department of Chemical and Biomolecular Engineering National University of SingaporeSingapore Department of Respiratory Medicine Jinling HospitalNanjingJiangsu210002China

Complexing self-assembled dna nanostructures with various functional guest species is the key to unlocking new and exciting biomedical applications.Cationic guest species not only induce magnesium-free dna to self-assemble into defined structures but also endow the final complex nanomaterials with new properties.Herein,we propose a novel strategy that employs naturally occurring cationic amino acids to induce dna self-assembly into defined nanostructures.Natural L-arginine and L-lysine can readily induce the assembly of tile-based dna nanotubes and dna origami sheets in a magnesium-free manner.The self-assembly processes are demonstrated to be pH-and concentration-dependent and are achieved at constant temperatures.Moreover,the assembled dna/amino acid complex nanomaterials are stable at a physiological temperature of 37◦C.Substituting L-arginine with its D form enhances its serum stability.Further preliminary examination of this complex nanomaterial platform for biomedical applications indicates that dna/amino acids exhibit distinct cellular uptake behaviors compared with their magnesium-assembled counterparts.The nanomaterial mainly clusters around the cell membrane and might be utilized to manipulate molecular events on the membrane.Our study suggests that the properties of dna nanostructures can be tuned by complexing them with customized guest molecules for a designed application.The strategy proposed herein might be promising to advance the biomedical applications of dna nanostructures.

关键词： dna nanostructures Noncanonical dna self-Assembly Amino acids Isothermal self-assembly

Pharmaceutical applications of framework nucleic acids

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Acta Pharmaceutica Sinica B 2022年第1期12卷 76-91页

作者： Liang Chen Jie Zhang Zhun Lin Ziyan Zhang Miao Mao Jiacheng Wu Qian Li Yuanqing Zhang Chunhai Fan School of Pharmaceutical Sciences Sun Yat-sen UniversityGuangzhou 510006China School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules and National Center for Translational MedicineShanghai Jiao Tong UniversityShanghai 200240China Institute of Molecular Medicine Shanghai Key Laboratory for Nucleic Acids Chemistry and NanomedicineRenji HospitalSchool of MedicineShanghai Jiao Tong UniversityShanghai 200127China

dna is a biological polymer that encodes and stores genetic information in all living organism. Particularly, the precise nucleobase pairing inside dna is exploited for the self-assembling of nanostructures with defined size, shape and functionality. These dna nanostructures are known as framework nucleic acids(FNAs) for their skeleton-like features. Recently, FNAs have been explored in various fields ranging from physics, chemistry to biology. In this review, we mainly focus on the recent progress of FNAs in a pharmaceutical perspective. We summarize the advantages and applications of FNAs for drug discovery, drug delivery and drug analysis. We further discuss the drawbacks of FNAs and provide an outlook on the pharmaceutical research direction of FNAs in the future.

关键词： dna nanotechnology Self-assembly Framework nucleic acids dna nanostructures Drug discovery Therapeutic molecules Drug delivery Drug analysis

dna Nanostructure-Guided Plasmon Coupling Architectures

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CCS Chemistry 2023年第3期5卷 568-588页

作者： Mengmeng Liu Xiaoyu Zhang Lulu Huang Jie Li Chunhai Fan Yang Tian Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200241 School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesInstitute of Translational MedicineShanghai Jiao Tong UniversityShanghai 200240

Plasmon coupling architectures with specific spatial and orientational arrangement configurations possess unique and tailored plasmonic properties and hold promise for advancements in nano-optics,nanoantennas,and biosensors.Numerous research has focused on the construction of plasmonic assemblies with predetermined configurations.dna nanostructures with arbitrary geometry,high compatibility with metal nanoparticles,and spatial addressability meet the requirement for precise spatial and orientation arrangement.Currently,dna nanostructures are widely exploited as structural materials to generate plasmonic structures with well-defined topologies.We review the evolution of dna nanostructureguided plasmon coupling architectures,including the introduction of dna nanostructures,dna modification on the surface of plasmonic nanoparticles,and three strategies for constructing complex plasmonic nanostructures.Then we focus on the emerging applications of dna nanostructure-guided architectures with engineered local electromagnetic enhancement for modulating plasmon coupling,amplifying emitter signals,and serving as biosensors.Finally,we will critically discuss the challenges and opportunities in this field.

关键词： dna nanostructures plasmonic nanoparticles localized surface plasmon resonance plasmon coupling architectures

Framework nucleic acid-based confined enzyme cascade for efficient synergistic cancer therapy in vivo

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Science China Chemistry 2021年第4期64卷 660-665页

作者： Gezhi Kong Meng Zhang Mengyi Xiong Mei Chen Chan Yang Yan Zhao Yue Yang Zilong Zhao Zhi-Ling Song Liang Gong Guoliang Ke Xiao-Bing Zhang Weihong Tan Molecular Science and Biomedicine Laboratory State Key Laboratory of Chemo/Biosensing and ChemometricsCollege of Chemistry and Chemical EngineeringCollaborative Innovation Center for Chemistry and Molecular MedicineHunan UniversityChangsha 410082China College of Materials Science and Engineering Hunan UniversityChangsha 410082China Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science Ministry of Education/Shandong Key Laboratory of Biochemical Analysis/College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China Hunan Key Laboratory of Biomedical Nanomaterials and Devices College of Life Sciences and ChemistryHunan University of TechnologyZhuzhou 412007China

Artificial enzyme cascade systems with confinement effect are highly important in synthetic biology and biomedicine.Herein,a framework nucleic acid-based confined enzyme cascade(FNA-CEC)for synergistic cancer therapy in vivo was developed.The FNA-CEC consisted of glucose oxidase and horseradish peroxidase precisely assembled on an addressable dna tetrahedron scaffold within few nanometers.Glucose oxidase(GOx)can trigger efficient glucose depletion for tumor starvation therapy,and increase the local concentration of H_(2)O_(2) in situ for enhanced downstream horseradish peroxidase(HRP)-activated prodrug therapy.Due to the spatial-confinement on dna tetrahedron scaffold,the efficiency of intermediate metabolites transportation between the enzyme cascades was improved.Moreover,FNA-CEC was applied for efficient synergistic cancer therapy in vitro and in vivo.As a simple and efficient approach,the FNA-CEC is expected to expand the toolbox of technologies in synthetic biology and biomedicine.

关键词： dna nanotechnology dna nanostructures drug delivery enzyme cascade cancer therapy

Biomacromolecular nanostructures-based interfacial engineering: from precise assembly to precision biosensing

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National Science Review 2018年第5期5卷 740-755页

作者： Fan Yang Xiaolei Zuo Chunhai Fan Xian-En Zhang Division of Physical Biology & Bioimaging Center Shanghai Synchrotron Radiation FacilityShanghai Institute of Applied PhysicsChinese Academy of Sciences National Key Laboratory of Biomacromolecules CAS Excellence Center for BiomacromoleculesInstitute of BiophysicsChinese Academy of Sciences School of Laboratory Medicine Hubei University of Chinese Medicine

Biosensors are a type of important biodevice that integrate biological recognition elements, such as enzyme,antibody and dna, and physical or chemical transducers, which have revolutionized clinical diagnosis especially under the context of point-of-care tests. Since the performance of a biosensor depends largely on the bio–solid interface, design and engineering of the interface play a pivotal role in developing quality biosensors. Along this line, a number of strategies have been developed to improve the homogeneity of the interface or the precision in regulating the interactions between biomolecules and the interface. Especially,intense efforts have been devoted to controlling the surface chemistry, orientation of immobilization,molecular conformation and packing density of surface-confined biomolecular probes(proteins and nucleic acids). By finely tuning these surface properties, through either gene manipulation or self-assembly, one may reduce the heterogeneity of self-assembled monolayers, increase the accessibility of target molecules and decrease the binding energy barrier to realize high sensitivity and specificity. In this review, we summarize recent progress in interfacial engineering of biosensors with particular focus on the use of protein and dna nanostructures. These biomacromolecular nanostructures with atomistic precision lead to highly regulated interfacial assemblies at the nanoscale. We further describe the potential use of the high-performance biosensors for precision diagnostics.

关键词： biosensor interface engineering homogeneity orientation control fused proteins dna nanostructures

Functional dna Structures and Their Biomedical Applications

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CCS Chemistry 2020年第5期2卷 707-728页

作者： Ziyuan Li Chen Wang Jiang Li Junji Zhang Chunhai Fan Itamar Willner He Tian Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterSchool of Chemistry and Molecular EngineeringEast China University of Science&TechnologyShanghai 200237(China) Institute of Chemistry The Minerva Center for Biohybrid Complex SystemsThe Hebrew University of JerusalemJerusalem 91904(Israel) Bioimaging Center Shanghai Synchrotron Radiation FacilityZhangjiang LaboratoryShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210(China) School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai 200240(China)

Since the discovery of the double-helix structure in 1953,nucleic acids have been developed from natural genetic codes into functional building blocks in a wide range of biotechnology and materials sciences.Taking advantage of their design diversity and biocompatibility,functional nucleic acids facilitate the“bottom-up”fabrication of nanomaterials that are highly potential for molecular medicine to treat different diseases,such as cancers.The present perspective article introduces recent advances in the use of these unique properties of nucleic acid biopolymers for biomedical applications.Specifically,nanomaterial/nucleic acid hybrid structures for sensing,controlled drug release,programmable intracellular imaging,and apoptosis,as well as logic calculation,are discussed.Furthermore,the detailed operation for both extracellular and intracellular bioactivity regulation with these new design functional nucleic acid nanostructures are fully illustrated.

关键词： nucleic acid nanomaterial/dna hybrid dna nanostructures dna logic cell regulation