Enzyme-Free Dynamic DNA Reaction Networks for On-Demand Bioanalysis and Bioimaging DOI
Shizhen He,

Jinhua Shang,

Yuqiu He

et al.

Accounts of Chemical Research, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 25, 2024

ConspectusThe pursuit of in-depth studying the nature and law life activity has been dominating current research fields, ranging from fundamental biological studies to applications that concern synthetic biology, bioanalysis, clinical diagnosis. Motivated by this intention, spatiotemporally controlled in situ analysis living cells a prospective branch virtue high-sensitivity imaging key biomolecules, such as biomarkers. The past decades have attested deoxyribonucleic acid (DNA), with biocompatibility, programmability, customizable features, is competitive biomaterial for constructing high-performance molecular sensing tools. To conquer complexity wide extracellular–intracellular distribution biomarkers, it meaningful breakthrough explore high-efficiently amplified DNA circuits, which excel at operating complex yet captivating dynamic reaction networks various bioapplications. In parallel, multidimensional performance improvements nucleic including availability, detection sensitivity, reliability, are critical parameters realizing accurate cell regulation bioanalysis.In Account, we summarize our recent work on enzyme-free bioanalysis three main aspects: circuitry functional extension recognition epigenetic regulation, amplification ability improvement sensitive biomarker detection, site-specific activation systems reliable imaging. first part, designed an epigenetically responsive deoxyribozyme (DNAzyme) system intracellular gene enriches possible analyzed species chemically modifying conventional DNAzyme. For example, exquisite N6-methyladenine (m6A)-caged DNAzyme was built achieving precise FTO (fat mass obesity-associated protein)-directed regulation. addition, varieties DNAzyme-based nanoplatforms self-sufficient cofactor suppliers were assembled, subdued speed-limiting hardness cofactors live-cell applications. second developed series hierarchically assembled improve signal transduction traditional circuits. First, circuit significantly enhanced via several heterogeneously or homogeneously concatenated models. Furthermore, feedback pathway integrated into these thus dramatically increasing efficiency. Second, considering cellular environment, simplified redundancy multicomponents procedures cascaded relying minimal component merely one modular catalytic reaction, guaranteed high cell-delivering uniformity while fostering kinetics reliability. third constructed in-cell-selective endogenous-stimulated multiply recognitions, could not only eliminate leakage, but also retain its on-site multiplex amplification. Based strategy, more availability scenarios acquired These demonstrate purpose-to-concreteness engineering tailored multimolecule multiple amplification, high-gain high-reliability targeted bioanalysis. We envision network can contribute bioanalytical layouts, will facilitate progression diagnosis prognosis.

Language: Английский

Near-Infrared Light Controllable DNA Walker Driven by Endogenous Adenosine Triphosphate for in Situ Spatiotemporal Imaging of Intracellular MicroRNA DOI

Mingqiang Ye,

Yujing Kong,

Cuiling Zhang

et al.

ACS Nano, Journal Year: 2021, Volume and Issue: 15(9), P. 14253 - 14262

Published: Aug. 19, 2021

As a powerful signal amplification tool, the DNA walker has been widely applied to detect rare microRNA (miRNA) in vivo. Despite significant advances, near-infrared (NIR) light controllable for powered by an endogenous initiator not realized, which is crucial spatiotemporal imaging of miRNA living cells with high sensitivity. Herein, we constructed NIR-photoactivatable system, was adenosine triphosphate (ATP) situ spatial and temporal resolution. The system very stable extremely low fluorescent background bioimaging cells. We employed upconversion nanoparticles (UCNPs) as carriers probe transducers converting NIR UV light. Coupled fueled intracellular ATP, smart based on initiated successfully developed precise control Triggered light, could autonomously progressively travel along track assistance ATP. different cell lines highly This strategy can expand photocontrol biological system.

Language: Английский

Citations

111

Spatially Selective Imaging of Mitochondrial MicroRNAs via Optically Programmable Strand Displacement Reactions DOI
Jian Zhao, Zhixiang Li,

Yulei Shao

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(33), P. 17937 - 17941

Published: June 12, 2021

Abstract MicroRNA (miRNA) functions are tightly regulated by their sub‐compartmental location in living cells, and the ability to imaging of mitochondrial miRNAs (mitomiRs) is essential for understanding related pathological processes. However, most existing DNA‐based methods could not be used this purpose. Here, we report development a DNA nanoreporter technology mitomiRs cells through near‐infrared (NIR) light‐controlled strand displacement reactions. The sensing function nanoreporters silent (OFF) during delivery process, but can photoactivated (ON) with NIR light after targeted localization, enabling spatially‐restricted two types cancer‐related improved detection accuracy. Furthermore, demonstrate vivo spatiotemporally‐controlled activation. Therefore, study illustrates simple methodology that may broadly applicable investigating mitomiRs‐associated physiological events.

Language: Английский

Citations

107

On‐Site Non‐enzymatic Orthogonal Activation of a Catalytic DNA Circuit for Self‐Reinforced In Vivo MicroRNA Imaging DOI
Shizhen He, Shanshan Yu, Ruomeng Li

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(45)

Published: July 1, 2022

Abstract The wide extracellular‐intracellular distribution of microRNA requires the on‐site, robust and efficient activation catalytic DNA circuits inside live cells. Herein, we develop an non‐enzymatic circuitry strategy to realize orthogonally controlled (CCD) circuit for achieving high‐fidelity in vivo imaging through multiply guaranteed molecular recognition progressively accelerated signal amplification. For predictable on‐site useful efficiency, dominating fuel strand was initially split into inactive subunits that were grafted auxiliary circuit. There, in‐cell‐specific mRNA triggered orthogonal amplification active strands sensitive target detection chief entropy‐driven We believe method can contribute clinical diagnosis prognosis.

Language: Английский

Citations

75

Photoactivation Inducing Multifunctional Coupling of Fluorophore for Efficient Tumor Therapy In Situ DOI
Weijie Zhang,

Yunxia Lv,

Fangjun Huo

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(23)

Published: Feb. 15, 2024

Abstract Photoactivatable molecules, with high‐precision spatialtemporal control, have largely promoted bioimaging and phototherapy applications of fluorescent dyes. Here, the first photoactivatable sensor ( BI ) is described that can be triggered by broad excitation light (405–660 nm), which further undergoes intersystem crossing H‐atom transfer processes to forming superoxide anion radicals (O 2 −• carbon radicals. Particularly, photoinduced gain carbon‐centered BI• allows for radical‐radical coupling afford combined crosslink product BI─BI ), would oxidized in presence O produce an extended conjugate system near infrared emission (820 nm). Besides, photochemically generated Cy─BI possesses ultra‐high photothermal conversion efficiency up 90.9%, optimized potential. What′s more, Western Blot assay reveals both photoproduct efficiently inhibit expression CHK1, irradiation induces apoptosis ultimately enhances phototherapeutic effects. Thus, combination cell cycle block inducing apoptosis, photodynamic therapy treatments significantly suppress solid tumor vivo antitumor efficacy explorations. This a novel finding developing as well applicability photoimaging tumor‐related areas.

Language: Английский

Citations

19

Photoactivatable Engineering of CRISPR/Cas9‐Inducible DNAzyme Probe for In Situ Imaging of Nuclear Zinc Ions DOI
Ran Liu,

Difei Jiang,

Yangfang Yun

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(10)

Published: Jan. 23, 2024

DNAzyme-based fluorescent probes for imaging metal ions in living cells have received much attention recently. However, employing situ within subcellular organelles, such as nucleus, remains a significant challenge. We developed three-stranded DNAzyme probe (TSDP) that contained 20-base-pair (20-bp) recognition site of CRISPR/Cas9, which blocks the activity. When Cas9, with its specialized nuclear localization function, forms an active complex sgRNA cell it cleaves TSDP at site, resulting formation catalytic structure. With this design, CRISPR/Cas9-inducible Zn

Language: Английский

Citations

17

Exogenously and Endogenously Sequential Regulation of DNA Nanodevices Enables Organelle‐Specific Signal Amplification in Subcellular ATP Profiling DOI Open Access
Xueyan Feng,

Deyu Yi,

Lele Li

et al.

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 9, 2025

Abstract Adenosine triphosphate (ATP), the primary energy currency in cells, is dynamically regulated across different subcellular compartments. The ATP interplay between mitochondria and endoplasmic reticulum (ER) underscores their coordinated roles various biochemical processes, highlighting necessity for precise profiling of dynamics. Here we present an exogenously endogenously dual‐regulated DNA nanodevice spatiotemporally selective, subcellular‐compartment specific signal amplification sensing. system allows exogenous NIR light‐controlled spatiotemporal localization activation aptamer sensor or ER, while a endogenous enzyme organelles further drives via consumption molecular beacon fuels, resulting significantly enhanced sensitivity spatial precision organelle interest. Furthermore, demonstrate application this robust monitoring fluctuations ER following drug interventions. This advancement provides powerful tool improving our understanding cellular energetics at level holds potential development targeted therapeutics.

Language: Английский

Citations

4

Tunable Organelle Imaging by Rational Design of Carbon Dots and Utilization of Uptake Pathways DOI

E Shuang,

Chuang He, Jianhua Wang

et al.

ACS Nano, Journal Year: 2021, Volume and Issue: 15(9), P. 14465 - 14474

Published: Sept. 9, 2021

Employing one-step hydrothermal treatment of o-phenylenediamine and lysine to exploit their self- copolymerization, four kinds CDs (ECDs, NCDs, GCDs, LCDs) are synthesized, possessing different surface groups (CH3, C–O–C, NH2, COOH) lipophilicity which endow them with various uptake pathways achieve tunable organelle imaging. Specifically, highly lipophilic ECDs CH3 group NCDs C–O–C select passive manner target endoplasmic reticulum nucleus, respectively. Amphiphilic GCDs CH3, NH2 prefer caveolin-mediated endocytosis locate at Golgi apparatus. Highly hydrophilic LCDs COOH involved in clathrin-mediated localize lysosomes. Besides, imaging results cell division, three-dimensional reconstruction living zebrafish demonstrate that the obtained promising potential candidates for specific organelle-targeting

Language: Английский

Citations

100

A Cooperatively Activatable, DNA‐based Fluorescent Reporter for Imaging of Correlated Enzymatic Activities DOI

Zetan Fan,

Jian Zhao, Xin Chai

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(27), P. 14887 - 14891

Published: April 19, 2021

The dynamic variation of the expression profile and spatial landscape multiple enzymes are crucial factors influencing tumor progression drug treatment. However, comprehensive analysis these events has been hampered by limitations existing imaging technologies. Here we report a cooperatively activatable, DNA-based fluorescent reporter programmed to detect correlated activity dual enzymes, telomerase (TE) apurinic/apyrimidinic endonuclease 1 (APE1), both in vitro vivo. conformational change DNA probe can be orthogonally triggered through TE-induced elongation APE1-mediated specific cleavage, producing signal for two an AND-gated manner. Furthermore, demonstrate capability system "dual lock-and-key" strategy, visualizing enzymatic activities during treatment cancer.

Language: Английский

Citations

92

Heterostructures Made of Upconversion Nanoparticles and Metal–Organic Frameworks for Biomedical Applications DOI
Qing Liu, Bo Wu, Mengyuan Li

et al.

Advanced Science, Journal Year: 2021, Volume and Issue: 9(3)

Published: Nov. 17, 2021

Abstract Heterostructure nanoparticles (NPs), constructed by two single‐component NPs with distinct nature and multifunctional properties, have attracted intensive interest in the past few years. Among them, heterostructures made of upconversion (UCNPs) metal–organic frameworks (MOFs) can not only integrate advantageous characteristics (e.g., porosity, structural regularity) MOFs unique upconverted optical features UCNPs, but also induce cooperative properties observed either for single component due to their special or electronic communications. Recently, diverse UCNP‐MOF are designed synthesized via different strategies demonstrated appealing potential applications biosensing imaging, drug delivery, photodynamic therapy (PDT). In this review, synthesis first summarized, then authors focus mainly on discussion biomedical applications, particularly as PDT agents cancer treatment. Finally, briefly outlook current challenges future perspectives hybrid nanocomposites. The believe that review will provide comprehensive understanding inspirations toward recent advances heterostructures.

Language: Английский

Citations

88

Recent Progress in DNA Hybridization Chain Reaction Strategies for Amplified Biosensing DOI
Hua Chai, Wenbo Cheng, Dayong Jin

et al.

ACS Applied Materials & Interfaces, Journal Year: 2021, Volume and Issue: 13(33), P. 38931 - 38946

Published: Aug. 10, 2021

With the continuous development of DNA nanotechnology, various spatial structures and assembly techniques emerge. Hybridization chain reaction (HCR) is a typical example with exciting features bright prospects in biosensing, which has been intensively investigated past decade. In this Spotlight on Applications, we summarize principles conventional HCR some novel forms linear/nonlinear HCR. advantages like great kinetics, facile operation, an enzyme-free isothermal reaction, these strategies can be integrated most mainstream reporters (e.g., fluorescence, electrochemistry, colorimetry) for ultrasensitive detection abundant targets. Particularly, select several representative studies to better illustrate ideas performances strategies. Theoretical practical utilities are confirmed range biosensing applications. end, deep discussion provided about challenges future tasks field.

Language: Английский

Citations

84