Ruthenium based metal–organic frameworks as annihilation electrochemiluminescence emitters coupled with DNA walker mediated signal amplification for sensitive detection of aflatoxin B1

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 159601 - 159601

Published: Jan. 1, 2025

Language: Английский

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Engineering DNA Nanodevices with Multi-site Recognition and Multi-signal Output for Accurate Intracellular LncRNA Imaging

Analytical Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 5, 2025

Dynamic DNA nanodevices, known for their high programmability and controllability, are pivotal in intracellular biomarker imaging. However, these nanodevices often suffer from inadequate detection sensitivity specificity due to limited cellular loading capacity low signal feedback. Herein, we engineered an integrated multi-site recognition multi-signal output of four-leaf clover dynamic nanodevice (MEMORY) that enables sensitive accurate long noncoding RNA (lncRNA) MEMORY features one fluorophore (FAM)-modified cross-shaped structure as spatial-confinement scaffolds loaded with four identical quenchers (BHQ1)-modified probes (RPs), ensuring a background initially. In the presence target lncRNA, multiple sites facilitate hybridization selectively release RPs, exposing toehold region outputting green fluorescence (FAM) signal. Furthermore, exposed can trigger efficient rapid chain reaction (HCR) amplification, red (Cy5) MEMORY's increase likelihood collisions, enhancing efficiency, while its provides sequential feedback through FAM Cy5, boosting overall intensity. With lncRNA metastasis-related lung adenocarcinoma transcript 1 (MALAT1) model, offers linear range pM 100 nM, limit 0.29 pM. We demonstrated differentiate between normal tumor cells based on MALAT1 This will offer valuable tools imaging biomarkers.

Language: Английский

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Steric Engineering of Perylene Derivative Side Chains To Boost Electrochemiluminescence for High-Performance Bioanalysis

Analytical Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: April 20, 2025

Traditional organic planar aromatic emitters often encounter low electrochemiluminescence (ECL) efficiency due to the aggregation-induced quenching (ACQ) induced by π-π stacking, limiting their applicability in bioanalysis. In this work, we proposed a steric engineering strategy mitigate ACQ perylene diimide-bridged β-cyclodextrin aggregates (Pe-CD aggregates), significantly boosting ECL for trace microRNA (miRNA) detection. By incorporation of large volume cyclic (β-CD) at both side chains diimide, Pe-CD molecules were generated and further assembled into robust supramolecular nanoblocks. This modulates intermolecular distances around cores, effectively minimizing nonradiative relaxation. Molecular simulation results demonstrated that distance increased from 3.32 Å 5.21 Å, accompanied 5.8-fold enhancement compared Pe (formed dense stacking molecules). As proof concept, an bioassay platform was developed using as target-enrichment accelerated-3D DNAzyme walkers signal amplifiers detecting miRNA-21, achieving limit detection 9.7 aM. study offers valuable insights designing new expands potential applications technology.

Language: Английский

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Programmable Split DNAzyme Modulators via Allosteric Cooperative Activation for mRNA Electrochemiluminescence Biosensing

Analytical Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: March 3, 2025

DNAzymes, known for their programmability, stability, and cost-effectiveness, are powerful tools signal transduction in complex biological systems. However, application responding to target effectors is often hindered by limited catalytic efficiency susceptibility unintended activation. Here we propose an allosteric cooperative activation strategy program a split DNAzyme modulator (STATER) that enables sensitive accurate electrochemiluminescence (ECL) biosensing of interleukin-6 (IL-6) mRNA. Our design features STATER leverages DNA tetrahedron as central scaffold, equipped with two pairs T-shaped hairpin probes (TP) helper (HP). Specifically, the TP contains apurinic/apyrimidinic endonuclease 1 (APE1) recognition sites, IL-6 mRNA region, partzyme fragment, while HP corresponding paired fragment. Unlike conventional modulators rely on single effector activation, integrates mechanism, which ensures all preblocked components synergistically activated assembled within confined space, facilitating rapid specific reconstruction DNAzyme's active domain. Furthermore, upon APE1 mRNA, inactive partzymes undergo assembly via toehold exchange displacement reaction, switching cleavage reactivity STATER. This mechanism establishment threshold thereby minimizing nonspecific scenarios. studies demonstrate exhibits outstanding sensitivity selectivity detection using supramolecular gold nanoclusters network-based ECL platform. The biosensor provides linear span from × 10–13 10–7 M, limit low 3.26 10–14 highlighting STATER's potential detecting various analytes

Language: Английский

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Programmable spherical nucleic acids integrated with MOF-confined copper nanoclusters facilitate electrochemiluminescence detection of prostate-specific biomarkers

Journal of Materials Chemistry B, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

The designed all-in-one SNAs anchored with ice-cream probes achieve three functions: (i) enhanced AMACR conversion efficiency; (ii) promoted rolling circle amplification and (iii) improved CRISPR/Cas12a activation efficiency.

Language: Английский

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An engineered tweezer-shaped DNA generator to activate Cas12a via auto-cycling proximity recording amplification for APE1 activity assay

Sensors and Actuators B Chemical, Journal Year: 2024, Volume and Issue: unknown, P. 137145 - 137145

Published: Dec. 1, 2024

Language: Английский

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Specific Response Assembly of 3D Space-Confined DNA Nanoaggregates for Rapid and Sensitive Detection of DNA Methyltransferase

Analytical Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 18, 2024

Rapid and sensitive detection of DNA adenine methyltransferase (Dam) activity is crucial for both research clinical applications. Herein, we utilize two types spherical nucleic acids (SNAs) to specific response assemble into 3D space-confined nanoaggregates that enable the rapid Dam activity. The SNAs feature order scaffolds serve as cores anchoring signal hairpin probes (S-HPs) target (T-HPs). Specifically, distinct S-HPs are labeled with FAM fluorophores BHQ1 quenchers share identical sequences, while T-HPs designed different linking sequences recognition regions, resulting in formation (SNA1 SNA2). In presence Dam, region methylated subsequently cleaved by auxiliary endonuclease, releasing loop T-HP a walking strand exposing sequence on SNAs. Notably, prior design complementary facilitates their assembly nanoaggregates, creating confined space strands recover fluorescent signals. nanoaggregate system not only provides highly ordered tracks but also enhances spatial continuity strands, greatly improving reaction kinetics detecting This strategy enables within 105 min, achieving limit 2.9 × 10

Language: Английский

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DNA lesion-gated dumbbell nanodevices enable on-demand activation of the cGAS-STING pathway for enhancing cancer immunotherapy

Chemical Science, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 23, 2024

We developed a uracil base lesion-gated dumbbell DNA nanodevice (UBLE) that allows on-demand activation and termination of the cGAS-STING pathway in tumor cells, affording precise reliable avenue to enhance cancer immunotherapy.

Language: Английский

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