Programmable Entropy-Driven Circuit-Cascaded Self-Feedback DNAzyme Network for Ultra-Sensitive Fluorescence and Photoelectrochemical Dual-Mode Biosensing

Analytical Chemistry, Journal Year: 2024, Volume and Issue: 96(18), P. 7274 - 7280

Published: April 24, 2024

Inspired by natural DNA networks, programmable artificial networks have become an attractive tool for developing high-performance biosensors. However, there is still a lot of room expansion in terms sensitivity, atom economy, and result self-validation current microRNA sensors. In this protocol, miRNA-122 as target model, ultrasensitive fluorescence (FL) photoelectrochemical (PEC) dual-mode biosensing platform developed using entropy-driven circuit (EDC) cascaded self-feedback DNAzyme network. The well-designed EDC realizes full utilization the strands improves atomic economy signal amplification system. unique rational design double-CdSe quantum-dot-released substrate network significantly avoids high background signals enhances sensitivity specificity. Also, enzyme-free, effectively risk leakage accuracy sensor. Moreover, introduction superparamagnetic Fe

Language: Английский

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Shaping the Future of the Neurotransmitter Sensor: Tailored CdS Nanostructures for State-of-the-Art Self-Powered Photoelectrochemical Devices

ACS Sensors, Journal Year: 2024, Volume and Issue: 9(5), P. 2684 - 2694

Published: May 2, 2024

Semiconductor-based photoelectrochemical (PEC) test protocols offer a viable solution for developing efficient individual health monitoring by converting light and chemical energy into electrical signals. However, slow reaction kinetics electron–hole complexation at the interface limit their practical application. Here, we reported triple-engineered CdS nanohierarchical structures (CdS NHs) modification scheme including morphology, defective states, heterogeneous structure to achieve precise of neurotransmitter dopamine (DA) in plasma noninvasive body fluids. By precisely manipulating Cd–S precursor, achieved control over ternary NHs obtained well-defined layered self-assembled through surface carbon treatment. The integration defect states thin layer effectively established carrier directional transfer pathways, thereby enhancing sites improving conversion efficiency. microelectrode fabricated demonstrated remarkable negative response toward DA, enabling development miniature self-powered PEC device quantification human saliva. Additionally, utilization density functional theory calculations elucidated structural characteristics DA state CdS, thus establishing crucial theoretical groundwork optimizing polymerization process DA. present study offers potential engineering approach high efficiency semiconductors as well proposing novel concept designing sensitive testing strategies.

Language: Английский

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In Situ Cascade Catalytic Polymerization of Dopamine Based on Pt NPs/CoSAs@NC Nanoenzyme for Constructing Highly Sensitive Photocurrent‐Polarity‐Switching PEC Biosensing Platform

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 6, 2025

Nanozymes open up new avenues for amplifying signals in photoelectrochemical (PEC) biosensing, which are yet limited by the generated small-molecule signal reporters. Herein, a multifunctional nanoenzyme of Pt NPs/CoSAs@NC consisting Co single atoms on N-doped porous carbon decorated with nanoparticles is successfully synthesized cascade catalytic polymerization dopamine constructing highly sensitive photocurrent-polarity-switching PEC biosensing platform. Taking protein tyrosine phosphatase 1B (PTP1B) as target model, nanoenzymes linked to magnetic microspheres via phosphorylated peptides. Upon dephosphorylation PTP1B, multiple enzyme-like activities, including peroxidase (POD)-like, catalase (CAT)-like, and oxidase (OXD)-like released collected induce situ ZnCdS photoelectrode presence H

Language: Английский

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CRISPR/Cas13a-Programmed Cu NCs and Z-Scheme T-COF/Ag₂S for Photoelectrochemical Biosensing of circRNA

ACS Sensors, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 31, 2025

Circular RNAs (circRNAs), as a class of noncoding RNA molecules with circular structure exhibit high stability and spatiotemporal-specific expression, making them ideal cancer biomarkers for liquid biopsy. Herein, new photoelectrochemical (PEC) biosensor highly sensitive circRNA assay in the whole blood lung patients was designed based on CRISPR/Cas13a-programmed Cu nanoclusters (Cu NCs) Z-scheme covalent organic framework/silver sulfide (T-COF/Ag2S) composite. This T-COF/Ag2S composite accelerates electron transfer produces an excellent initial photocurrent. When CRISPR/Cas13a precisely targets circRNA, it nonspecifically cleaves triple-helix molecular to release DNA fragments (C'/C"). After C'/C" opens hairpin probe (HP) modified electrode, hybridization chain reactions are performed produce abundant AT-rich double-stranded addition H1 H2 probes. Upon incubation Cu2+, NCs situ formed via A-Cu2+-T bonds can effectively quench photocurrent due energy process. developed PEC shows low limit detection 0.5 fM, reusability DNA-modified magnetic beads (MB-DNA) reduces cost. Moreover, accurately quantify level distinguish expression from healthy controls patients, offering strong potential clinical diagnosis.

Language: Английский

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Enhanced Anti-Interference Photoelectrochemical DNA Bioassay: Grafting a Peptide-Conjugated Hairpin DNA Probe on a COF-Based Photocathode

ACS Sensors, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 6, 2025

Precise and sensitive analysis of specific DNA in actual human bodily fluids is crucial for the early diagnosis major diseases a deeper understanding functions. Herein, by grafting peptide-conjugated hairpin probe to covalent organic framework (COF)-based photocathode, robust anti-interference photoelectrochemical (PEC) bioassay was explored, which could specifically resist potential interference from nonspecific proteins reducing species. Human immunodeficiency virus (HIV) used as target (tDNA) PEC bioassay. The vinyl-functionalized COF (COF-V) modified with meso-tetra(4-carboxyphenyl)-porphine (TCPP) polydopamine (PDA) fabricate PDA/TCPP/COF-V served photocurrent signal transducer. Toward unconventional recognition element, (hDNA) efficiently linked linear zwitterionic peptide (LZP) form LZP-hDNA bioconjugate, then grafted onto COF-based photocathode. LZP generated sturdy interface on For tDNA probing, AgInS2 (AIS) quantum dots acted quenchers, marked signaling (sDNA) obtain AIS-sDNA labeling, striking drop achieved through λ-exonuclease (λ-Exo)-aided recycling. This novel endowed an impressive property without requiring tedious steps. By combining excellent photoelectric properties photocathode effective strategy, accurate results probing were achieved.

Language: Английский

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Advanced Dual-Mode Microfluidic Sensing Platform Based on Amphiphilic Polymer-Capped Perovskite Nanozymes Induced Photoelectrochemical Signal Amplification and Fluorescence Emission

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

Published: Jan. 9, 2025

A novel dual-mode microfluidic sensing platform integrating photoelectrochemical (PEC) and fluorescence (FL) sensors was developed for the sensitive monitoring of heart fatty acid binding protein (h-FABP). First, BiVO4/AgInS2 (BVAIS) composites with excellent photoelectric activity were synthesized as matrices. The BVAIS heterojunction a well-matched internal energy level structure provided stable photocurrent. Second, an innovative signal amplification strategy based on octylamine-modified poly(acrylic acid) (OPA)-capped CsPbBr3 (OPCB) nanocrystals (NCs) catalytic property proposed. On OPCB nanozyme possessing ascorbate oxidase-like could catalyze oxidation ascorbic acid, which achieved quenching photocurrent signals by competitively consuming electron donor. other hand, NCs that overcame water stability defect processed good luminescence performance able to produce obvious FL signals. Mutually verified dual-response effectively enhance precision test outcomes avoid false-positive or false-negative results. Finally, constructed realized detection h-FABP in linear range 0.0001–150 ng/mL (PEC mode) 0.001–150 (FL mode), limits 36 fg/mL 0.32 pg/mL, respectively. present work new perspective designing efficient achieve disease markers.

Language: Английский

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Polydopamine Enhanced Interactions of Graphene Nanosheets to Fabricate Graphene/Polydopamine Aerogels with Effectively Clear Organic Pollutants

Langmuir, Journal Year: 2024, Volume and Issue: 40(18), P. 9592 - 9601

Published: April 22, 2024

Graphene/polydopamine aerogels (GPDXAG, where X represents the weight ratio of DA·HCl to GO) were prepared by chemical reduction graphene oxide (GO) using dopamine (DA) and l-ascorbic acid as reducing agents. During gelation process, DA was polymerized form polydopamine (PDA). The introduction PDA in led a deeper GO stronger interactions between nanosheets forced covalent cross-linking noncovalent bonding including π–π stacking hydrogen bonding. influencing formation morphology GPDXAG explored. With increasing content gelation, degree enhanced, resulting had more regular pore distribution. Additionally, introducing into improved its hydrophobicity because adhesion network aerogels. exhibited higher removal efficiency for organic pollutants than controlled (GAG). Specifically, adsorption capacity solvents superior that GAG, solvent completely separated from oil/water mixture GPDXAG. equilibrium malachite green (MG) measured be 768.50 mg/g, which methyl orange (MO). In MG/MO mixed solutions, obvious selectivity cationic dye. mechanism MG also discussed simulating kinetic models isothermal models.

Language: Английский

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AgI Precipitation Induced Polarity Reversal with Formation of Z-Type Heterojunction for Photoelectrochemical Sensing

Analytical Chemistry, Journal Year: 2024, Volume and Issue: 96(37), P. 14759 - 14765

Published: Sept. 5, 2024

Regulating photocurrent polarity is highly attractive for fabricating photoelectrochemical (PEC) biosensors with improved sensitivity and accuracy in practical samples. Here, a new approach that adopts the situ generated AgI precipitate AgNCs to reversal Bi

Language: Английский

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Enhancement in Photo-Response of CuZnS Nanocrystals-Based Photodetector Using Asymmetric Work Function Electrodes

Optical Materials, Journal Year: 2024, Volume and Issue: unknown, P. 116182 - 116182

Published: Sept. 1, 2024

Language: Английский

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Near-infrared light-driven polypyrrole/UiO-66-NH2 n-n heterojunction enabled paper-based photoelectrochemical aptasensing of bis(2-ethylhexyl) phthalate

Microchemical Journal, Journal Year: 2025, Volume and Issue: unknown, P. 113452 - 113452

Published: March 1, 2025

Language: Английский

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