Flexible Self-Powered Sensing System Based on Novel DNA Circuit Strategy and Graphdiyne for Thalassemia Gene by Rapid Naked-Eye Tracking and Open-Circuit Voltage

Analytical Chemistry, Год журнала: 2023, Номер 95(44), С. 16374 - 16382

Опубликована: Окт. 23, 2023

Based on the controllable instantaneous self-assembly ability of long-chain branched DNA nanostructures and synergistic effect between nucleic acid amplification without enzymes, a highly sensitive specific self-powered biosensing platform is developed. Two-dimensional graphdiyne prepared, modified flexible carbon cloth, then functionalized with gold nanoparticles. When mi-tubes are applied it, target thalassemia gene CD122 triggers dual-catalytic hairpin assembly reaction. The generated nanoscale precisely captured by mi-tube, exposing binding sites activating hybridization chain reaction to form DNA. Double-stranded DNA, along dendritic carrying large number guanine bases, captures signal molecule methylene blue (MB), generating significant electrochemical signal. redox MB also causes proportional change in system's color, achieving colorimetric detection functionality. An efficient dual-mode sensing platform, therefore, established for detecting CD122. linear response range concentration open-circuit voltage RGB Blue value 0.0001–10,000 pM. limit under mode 36.3 aM (S/N = 3), mode, it as low 12.1 3). new method exhibits high sensitivity, excellent selectivity, accuracy, providing universal strategy designing novel platforms that can be extended other biomolecules.

Язык: Английский

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A Smart Deoxyribozyme‐Programmable Catalytic DNA Circuit for High‐Contrast MicroRNA Imaging

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(33)

Опубликована: Июнь 28, 2023

Synthetic catalytic DNA circuits have been recognized as a promising signal amplification toolbox for sensitive intracellular imaging, yet their selectivity and efficiency are always constrained by uncontrolled off-site leakage inefficient on-site circuitry activation. Thus, the endogenously controllable exposure/activation of is highly desirable achieving selective imaging live cells. Herein, an activated DNAzyme strategy was facilely integrated with circuit guiding efficient microRNA in vivo. To prevent activation, constitute initially caged without sensing functions, which could be selectively liberated amplifier to guarantee high-contrast target This intelligent modulation can tremendously expand these molecularly engineered biological systems.

Язык: Английский

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DNA as a universal chemical substrate for computing and data storage

Nature Reviews Chemistry, Год журнала: 2024, Номер 8(3), С. 179 - 194

Опубликована: Фев. 9, 2024

Язык: Английский

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DNAzyme-Based Dissipative DNA Strand Displacement for Constructing Temporal Logic Gates

ACS Nano, Год журнала: 2024, Номер 18(3), С. 2184 - 2194

Опубликована: Янв. 9, 2024

Toehold-mediated DNA strand displacement is the foundation of dynamic nanotechnology, encompassing a wide range tools with diverse functions, dynamics, and thermodynamic properties. However, majority these are limited to unidirectional reactions driven by thermodynamics. In response growing field dissipative we present an approach: DNAzyme-based (D-DSD), which combines principles nanotechnology nanotechnology. D-DSD introduces circular characteristics, distinguishing it from observed in conventional displacement. We investigated reaction mechanism devised temporal control elements. By substituting components, designed two distinct AND gates using fewer than 10 strands, eliminating need for complex network designs. contrast previous logic gates, our storage not through dynamics or cross-inhibition but autoregressive storage, more modular scalable approach memory storage. preserves fundamental structure toehold-mediated displacement, while offering enhanced simplicity versatility.

Язык: Английский

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Dynamic Near‐Infrared Circularly Polarized Luminescence Encoded by Transient Supramolecular Chiral Assemblies

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(32)

Опубликована: Май 13, 2024

Abstract Circularly polarized luminescence (CPL) is promising for applications in many fields. However, most systems involving CPL are within the visible range; near‐infrared (NIR) CPL‐active materials, especially those that exhibit high g lum values and can be controlled spatially temporally, rare. Herein, dynamic NIR‐CPL with a value of 2.5×10 −2 was achieved through supramolecular coassembly energy‐transfer strategies. The chiral assemblies formed by between adenosine triphosphate (ATP) pyrene derivative exhibited red signal ( 10 −3 ). further introduction sulfo‐cyanine5 resulted process, which not only led to NIR but also increased . Temporal control these realized introducing alkaline phosphatase fabricate biomimetic enzyme‐catalyzed network, allowing turned on. Based on enzyme‐regulated temporally controllable assemblies, multilevel information encryption system developed. This study provides pioneering example construction materials ability perform temporal via assembly strategy, expected aid design complex more closely resemble natural biological systems.

Язык: Английский

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Efficient Delivery of Lomitapide using Hybrid Membrane‐Coated Tetrahedral DNA Nanostructures for Glioblastoma Therapy

Advanced Materials, Год журнала: 2024, Номер 36(24)

Опубликована: Апрель 3, 2024

Abstract Glioblastoma (GBM) is the most aggressive and prevalent primary malignant tumor of central nervous system. Traditional chemotherapy has poor therapeutic effects significant side due to drug resistance, natural blood‐brain barrier (BBB), nonspecific distribution, leading a lack clinically effective drugs. Here, 1430 small molecule compounds are screened based on high‐throughput screening platform novel anti‐GBM drug, lomitapide (LMP) obtained. Furthermore, bionic nanodrug delivery system (RFA NPs) actively targeting GBM constructed, which mainly consists tetrahedral DNA nanocages (tFNA loaded with LMP as core folate‐modified erythrocyte–cancer cell–macrophage hybrid membrane (FRUR) shell. FRUR camouflage conferred unique features tFNA NPs, including excellent biocompatibility, improved pharmacokinetic profile, efficient BBB permeability, ability. The results show that RFA NPs exhibited superior specific activities, reduced off‐target delivery, prolonged lifespan, negligible in tumor‐bearing mice. This study combines biomimetic technology provide theoretical practical basis for development optimization clinical treatment strategies treatment.

Язык: Английский

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Orthogonal Enzyme-Driven Timers for DNA Strand Displacement Reactions

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(43), С. 19791 - 19798

Опубликована: Окт. 18, 2022

Here, we demonstrate a strategy to rationally program delayed onset of toehold-mediated DNA strand displacement reactions (SDRs). The approach is based on blocker strands that efficiently inhibit the by binding toehold domain target DNA. Specific enzymatic degradation subsequently enables SDR. kinetics thus controls time at which SDR starts. By varying concentration and enzyme, show can finely tune modulate Additionally, versatile be orthogonally controlled different enzymes each specifically targeting strand. We designed established three SDRs using RNase H two repair (formamidopyrimidine glycosylase uracil-DNA glycosylase) corresponding blockers. achieved temporal delay programed with high flexibility without undesired leak conveniently predicted kinetic modeling. Finally, possible applications temporally control ligand release from nanodevice, inhibition protein aptamer, output signal generated logic circuit.

Язык: Английский

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Dissipative Systems Driven by the Decarboxylation of Activated Carboxylic Acids

Accounts of Chemical Research, Год журнала: 2023, Номер 56(7), С. 889 - 899

Опубликована: Март 14, 2023

ConspectusThe achievement of artificial systems capable being maintained in out-of-equilibrium states featuring functional properties is a main goal current chemical research. Absorption electromagnetic radiation or consumption species (a "chemical fuel") are the two strategies typically employed to reach such states, which have persist as long one above stimuli present. For this reason often referred "dissipative systems". In simplest scheme, dissipative system initially found resting, equilibrium state. The addition fuel causes shift an When exhausted, reverts initial, Thus, from mechanistic standpoint, turns out be catalyst for consumption. It has noted that, although very simple, scheme implies chance temporally control system. principle, modulating nature and/or amount added, can full time spent by state.In 2016, we that 2-cyano-2-phenylpropanoic acid (1a), whose decarboxylation proceeds smoothly under mild basic conditions, could used drive back and forth motion catenane-based molecular switch. donates proton catenane passes neutral state A transient protonated B. Decarboxylation resulting carboxylate (1acb), generates carbanion, which, strong base, retakes consequently, returns initial A. larger added fuel, longer transient, Since then, 1a other activated carboxylic acids (ACAs) been operation large number based on acid-base reaction, machines host-guest systems, catalysts smart materials, so on. This Account illustrates with purpose show wide applicability ACAs fuels. generality due simplicity idea underlying principle ACAs, always translates into simple experimental requirements.

Язык: Английский

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Mesoporous Nanozyme-Enhanced DNA Tetrahedron Electrochemiluminescent Biosensor with Three-Dimensional Walking Nanomotor-Mediated CRISPR/Cas12a for Ultrasensitive Detection of Exosomal microRNA

Analytical Chemistry, Год журнала: 2023, Номер 95(9), С. 4486 - 4495

Опубликована: Фев. 20, 2023

Exosomal microRNAs (exomiRNAs) have emerged as ideal biomarkers for early clinical diagnostics. The accurate detection of exomiRNAs plays a crucial role in facilitating applications. Herein, an ultrasensitive electrochemiluminescent (ECL) biosensor was constructed using three-dimensional (3D) walking nanomotor-mediated CRISPR/Cas12a and tetrahedral DNA nanostructures (TDNs)-modified nanoemitters (TCPP-Fe@HMUiO@Au-ABEI) exomiR-155 detection. Initially, the 3D strategy could effectively convert target into amplified biological signals improving sensitivity specificity. Then, TCPP-Fe@HMUiO@Au nanozymes with excellent catalytic performance were used to amplify ECL because enhanced mass transfer increased active sites, originating from its high surface areas (601.83 m2/g), average pore size (3.46 nm), large volumes (0.52 cm3/g). Meanwhile, TDNs scaffold fabricate "bottom-up" anchor bioprobes improve trans-cleavage efficiency Cas12a. Consequently, this achieved limit down 273.20 aM ranging 1.0 fM nM. Furthermore, discriminate breast cancer patients evidently by analyzing exomiR-155, these results conformed that qRT-PCR. Thus, work provides promising tool

Язык: Английский

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Dynamic Reconfigurable DNA Nanostructures, Networks and Materials

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(18)

Опубликована: Янв. 18, 2023

Abstract DNA nanotechnology relies on the structural and functional information encoded in nucleic acids. Specifically, sequence‐guided reconfiguration of acids by auxiliary triggers provides a means to develop switches, machines stimuli‐responsive materials. The present Review addresses recent advances construction applications dynamic reconfigurable nanostructures, networks Dynamic transformations proceeding within engineered origami frames or between tiles, triggered scaled supramolecular structures are addressed. use frameworks assemble chiroplasmonic optical devices operate switchable chemical processes discussed. Also, operation is addressed, design “smart” all‐DNA materials their introduced. Future perspectives nanostructures presented.

Язык: Английский

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