Emerging Data Processing Methods for Single‐Entity Electrochemistry

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(17)

Опубликована: Фев. 27, 2024

Single-entity electrochemistry is a powerful tool that enables the study of electrochemical processes at interfaces and provides insights into intrinsic chemical structural heterogeneities individual entities. Signal processing critical aspect single-entity measurements can be used for data recognition, classification, interpretation. In this review, we summarize recent five-year advances in signal techniques highlight their importance obtaining high-quality extracting effective features from signals, which are generally applicable electrochemistry. Moreover, shed light on noise analysis to obtain single-molecule frequency fingerprint spectra provide rich information about ion networks interface. By incorporating advanced tools artificial intelligence algorithms, would revolutionize field analysis, leading new fundamental discoveries.

Язык: Английский

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Single-Molecule Identification and Quantification of Steviol Glycosides with a Deep Learning-Powered Nanopore Sensor

ACS Nano, Год журнала: 2024, Номер 18(36), С. 25155 - 25169

Опубликована: Авг. 27, 2024

Steviol glycosides (SGs) are a class of high-potency noncalorie natural sweeteners made up common diterpenoid core and varying glycans. Thus, the diversity glycans in composition, linkage, isomerism results tremendous structural complexity SG family, which poses challenges for precise identification leads to fact that SGs frequently used mixtures their variances biological activity remain largely unexplored. Here we show wild-type aerolysin nanopore can detect discriminate diverse species through modulable electro-osmotic flow effect at varied applied voltages. At low voltages, neutral molecule was drawn stuck pore entrance due an energy barrier around R220 sites. The ensuing binding events enable majority species. Increasing voltage break cause translocation events, allowing unambiguous several pairs differing by only one hydroxyl group recognition accumulation from multiple sensing regions Based on data 15 SGs, deep learning-based artificial intelligence (AI) model created process individual blockage achieving rapid, automated, single-molecule quantification real samples. This work highlights value analysis complex glycans-containing glycosides, as well potential sensitive rapid quality assurance glycoside products with use AI.

Язык: Английский

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Electroanalytical systems based on solid-state nanochannel arrays for the detection of biomarkers of interest in clinical diagnostics

TrAC Trends in Analytical Chemistry, Год журнала: 2024, Номер 172, С. 117568 - 117568

Опубликована: Фев. 1, 2024

The stochastic sensing based on single nanopores is considered as one of the more relevant breakthroughs in bioanalysis, rightly summarized previous reviews. Inspired by it, use solid-state nanochannel arrays has paved way to electrochemical systems whose detection principle different that sensing. In view growing interest and continuous research improvements this field, an update much needed. Moreover, great potential these for clinical diagnostics deserves a special focus. context, review recent trends arrays-based electroanalytical biomarkers are presented. particular, we focus only prepared materials such alumina, silica, polyethylene terephthalate, titanium dioxide polystyrene nanospheres. Conclusions prospects future field also included.

Язык: Английский

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DNA–Peptide Interaction-Modulated Charge Reversal in Biomimetic Nanochannels for Simple and Efficient Detection of Histone Deacetylases

Analytical Chemistry, Год журнала: 2024, Номер 96(12), С. 4817 - 4824

Опубликована: Март 14, 2024

Protein acetylation, a fundamental post-translational modification, plays critical role in the regulation of gene expression and cellular processes. Monitoring histone deacetylases (HDACs) is important for understanding epigenetic dynamics advancing early diagnosis malignancies. Here, we leverage dynamic characteristics DNA–peptide interactions biomimetic nanochannels to develop HDAC detection method. In specific, catalysis peptide deacetylation by HDACs triggers alterations charge states nanochannel surface accommodate DNA molecules. Then, interaction between peptides shifts from positive negative, leading reversal ion current rectification (ICR). By calculation ICR ratio, quantitative can be efficiently achieved using nanochannel-based method an enzyme-free label-free manner. Our experimental results demonstrate that detected this within concentration range 0.5–500 nM. The innate simplicity efficiency strategy may render it valuable tool both research clinical applications realm epigenetics personalized medicine.

Язык: Английский

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A Portable Device for in Situ Noninvasive Monitoring of Cell Secretions and Communications with Fluorescence and Nanochannel Electrochemistry

Analytical Chemistry, Год журнала: 2024, Номер 96(22), С. 9218 - 9227

Опубликована: Май 23, 2024

In situ monitoring of cell secretions and communications plays a fundamental role in screening disease diagnostic biomarkers drugs. Quantitative detection intercellular communication have been separately reported, which often rely on target labeling or complex pretreatment steps, inevitably causing damage to the target. Simultaneous noninvasive are challenging never reported. Herein, we smartly developed portable device for label-free with fluorescence ion-transport-based nanochannel electrochemistry. Based dual signal mode, series nonelectroactive were sensitively accurately quantified. The limits VEGF, MUC1, ATP 3.84 pg/mL, 32.7 47.4 fM (3σ/S), 1/3.9, 1/1.1, 1/41 those commercial ELISA kits, respectively. More interestingly, under released secretions, gradual opening connected two cells left right chambers device; thus, secretion mediated can be monitored. proposed platform may provide promising tool understanding mechanism discovering new therapeutic targets.

Язык: Английский

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Superstructured Optoionic Heterojunctions for Promoting Ion Pumping Inspired by Photoreceptor Cells

ACS Nano, Год журнала: 2024, Номер 18(12), С. 9053 - 9062

Опубликована: Март 11, 2024

Photoreceptor cells of vertebrates feature ultrastructural membranes interspersed with abundant photosensitive ion pumps to boost signal generation and realize high gain in dim light. In light this, superstructured optoionic heterojunctions (SSOHs) cation-selective nanochannels are developed for manipulating photo-driven pumping. A template-directed bottom-up strategy is adopted sequentially assemble graphene oxide (GO) PEDOT:PSS into heterogeneous sculptured superstructures, which programmable variation membrane topography contain a donor–acceptor interface capable maintaining electron–hole separation upon photoillumination. Such elaborate design endows SSOHs much higher magnitude flux against concentration gradient contrast conventional planar configuration. This can be ascribed the buildup an enhanced transmembrane potential owing effective photogenerated carriers at heterojunction increase energy input from photoillumination due synergistic effect reflection reduction, broad-angle absorption, wide-waveband absorption. work unlocks significance topographies transportation proposes such universal prototype that could extended other develop high-performance artificial conversion sensing.

Язык: Английский

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Nanoprecipitation-Enhanced Sensitivity in Enzymatic Nanofluidic Biosensors

Analytical Chemistry, Год журнала: 2024, Номер 96(13), С. 5282 - 5288

Опубликована: Март 21, 2024

Single nanochannels show unique transport properties due to nanoconfinement. It has been demonstrated that at submillimolar concentrations of divalent cations, a nanoprecipitation reaction can occur in nanochannels. Although several reports have shown, described, and modeled the process, no further advantages taken from this phenomenon. Here, we be incorporated into enzyme-modified enhance performance small-molecule biosensors via situ amplification reactions. Contrary working principle previous enzymatic nanofluidic biosensors, biosensor described work operates on basis concerted functions: pH-shifting activity nanoprecipitation. We simple addition Ca2+ Mg2+ ions analyte solution containing urea lower detection limit nanometer subnanometer regime modulate dynamic linear range. This approach enables implementation more sensitive real-time methods without increasing complexity platform or sensing approach. envision integration functions architectures will play key role expanding use these nanoscale devices for analytical purposes.

Язык: Английский

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Orientational Pathways during Protein Translocation through Polymer-Modified Nanopores

ACS Nano, Год журнала: 2024, Номер 18(15), С. 10427 - 10438

Опубликована: Апрель 1, 2024

Protein translocation through nanopores holds significant promise for applications in biotechnology, biomolecular analysis, and medicine. However, the interpretation of signals generated by protein remains challenging. In this way, it is crucial to gain a comprehensive understanding on how macromolecules translocate nanopore identify what are critical parameters that govern process. study, we investigate interplay between charge regulation, orientation, surface modifications using theoretical framework allows us explicitly take into account acid–base reactions titrable amino acids proteins polyelectrolytes grafted surface. Our goal thoroughly characterize process different (GFP, β-lactoglobulin, lysozyme, RNase) modified with weak polyacids. calculations show regulation mechanism exerts profound effect The pH-dependent interactions charged polymers within lead diverse free energy landscapes barriers, wells, flat regions dictating efficiency. Comparison significance isoelectric point, size, morphology behavior. Taking advantage these insights, propose pH-responsive can load at one pH release them another, offering opportunities controlled delivery, separation, sensing applications.

Язык: Английский

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Super-assembled periodic mesoporous organosilica membranes with hierarchical channels for efficient glutathione sensing

The Analyst, Год журнала: 2024, Номер 149(13), С. 3522 - 3529

Опубликована: Янв. 1, 2024

A periodic mesoporous organosilica (PMO)-based heteromembrane with hierarchical pore architecture and glutathione (GSH)-responsive switchable wettability is synthesized for sensitive efficient GSH detection.

Язык: Английский

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Functional‐Nanochannel‐Based Artificial Postsynaptic Membrane for Neural Signal Transduction

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Авг. 9, 2024

Abstract Biological‐machine interface (BMI) devices represent a significant step toward adaptive and cognitive technologies. However, current BMI emphasize the analysis of electrophysiology often overlook chemical information neurotransmitters in process signaling between neurons. To bridge this gap, light‐gated artificial postsynaptic membrane (APM) is introduced, capable reading dopamine (DA) released from rat pheochromocytoma cells regulate neural signal transmission. Like biological membrane, APM porous functionalized by DA‐specific aptamers azobenzene (Azo) molecules different regions. Azo act as light‐responsive trigger that controls DA release, while capture DA, which converts its concentration into an ionic signal. By light‐enhanced responses to exocytosis (PC12) cells, confirms ability communicate with systems, lays foundation for developing biological‐machine interaction systems more advanced functionalities.

Язык: Английский

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