Boosting Microfluidic Enzymatic Cascade Reactions with pH‐Responsive Polymersomes by Spatio–Chemical Activity Control DOI Creative Commons

Andrea Koball,

Franziska Obst, Jens Gaitzsch

и другие.

Small Methods, Год журнала: 2024, Номер unknown

Опубликована: Июль 11, 2024

Abstract Microfluidic flow reactors permit the implementation of sensitive biocatalysts in polymeric environments (e.g., hydrogel dots), mimicking nature through use diverse microstructures within defined confinements. However, establishing complex hybrid structures to mimic biological processes and functions under continuous with optimal utilization all components involved reaction process represents a significant scientific challenge. To achieve spatial, chemical, temporal control for any microfluidic application, compartmentalization is required, as well unification different compartments chamber design. This study presents self‐regulating system fabricated by sequential photostructuring an intermediate chemical step realize pH‐sensitive fabrication double reactor controlled enzymatic cascade (ECR). The key point adaptation retention function pH‐responsive horseradish peroxidase‐loaded polymersomes chip flow. ECR successfully triggered interplay between glucose oxidase‐converted glucose, membrane state polymersomes, other parameters rate fluid composition). establishes promising noninvasive regulatory platform extended spatio–chemical current future systems.

Язык: Английский

Temporal pH waveforms generated in an enzymatic reaction network in batch and cell-sized microcompartments DOI Creative Commons
Masaki Itatani, Gábor Holló, Paola Albanese

и другие.

Cell Reports Physical Science, Год журнала: 2025, Номер unknown, С. 102367 - 102367

Опубликована: Янв. 1, 2025

Highlights•The emergent properties of the urease-esterase reaction network are investigated•The antagonistic enzymatic generates pH waveforms in batch•Front propagation and sol-gel transition fueled by network•One-cycle oscillation is realized giant unilamellar vesiclesSummaryInvestigating designing networks their phenomena backbone systems chemistry. Designing chemical oscillators homogeneous utilizing reactions challenging due to consumption substrates over one cycle. Here, we show that an comprising urea-urease ester-esterase can generate temporal variations a batch. We developed coupled kinetic model elucidate mechanism accurately captures experimentally observed variation time. To demonstrate remarkable potential network, expanded on this discovery generating front presenting several applications coupling fuel pH-dependent processes (gelation pH-sensitive monomers emulsion-vesicle transformation). By employing strategy reactions, engineered single pulse cell-sized microcompartments, which could contribute developing synthetic cells with multiple functions.Graphical abstract

Язык: Английский

Процитировано

1
Transient colloidal crystals fueled by electrochemical reaction products DOI Creative Commons

Medha Rath,

Satyam Srivastava, Eric A. Carmona

и другие.

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Фев. 28, 2025

Conventional electric field directed colloidal assembly enables fabricating ordered structures but lacks temporal control over state. Chemical reaction networks have been discovered that transiently assemble colloids; however, they slow dynamics (hrs – days) and poor tunability, utilize complex reagents, produce kinetically trapped states. Here we demonstrate transient crystals autonomously form, breakup, reconstitute in response to an electrochemical network driven by a time invariant electrical stimulus. Aqueous mixtures of micron sized colloids para-benzoquinone (BQ) were subjected superimposed oscillatory steady potentials, i.e., multimode induce electrokinetic flows around proton-coupled BQ redox reactions. Transient states coincided with electrochemically generated pH spikes near the cathode. We wide tunability state lifetimes two orders magnitude modifying potential electrode separation. An transport model showed interaction advancing acidic alkaline fronts from anodic oxidation cathodic reduction caused transients. present theoretical experimental evidence indicates mediated competition between opposing scale electrohydrodynamic electroosmotic flows, latter which is dependent. methods for struggle This study demonstrates disassemble, reassemble network, achieving using potentials.

Язык: Английский

Процитировано

0
Reactive Brownian Dynamics of Chemically Fueled Droplets: Roles of Attraction and Deactivation Modes DOI
Lennard Holschuh, Joachim Dzubiella

The Journal of Physical Chemistry B, Год журнала: 2025, Номер 129(2), С. 626 - 636

Опубликована: Янв. 6, 2025

The self-assembly of biological membraneless organelles can be mimicked by active droplets resulting from chemically fueled microphase separation. However, how the nonequilibrium, transient structure these controlled through physicochemical input parameters is not yet well understood. In our work, a two-state chemical reaction and subsequent droplet growth decay are modeled with reactive Brownian dynamics simulation in two spatial dimensions. model, particles that activated via consumption fuel become attractive accumulate into droplets. A local-density-dependent distinction droplet's 'internal' 'external' allows for structural feedback giving further control over deactivation process. shows only external slows down stabilizes droplets, whereas internal lead to temporary encapsulation deactivated (in nonequilibrium 'core–shell' structures) where serve as an outer shell. Additionally, role hydrophobicity resembled attraction energy ε dependency formation on various investigated. For example, high finite-size crystalline while other parameter choices indicate bimodal size distributions at specific times. Similarities differences related experiments discussed.

Язык: Английский

Процитировано

0
A Universal Strategy for Reversible and Spatiotemporal Electrofluorochromism of Eu3+ Metallogels Driven by Cooperative Chemical Reactions with Biomimetic Information “Memorizing‐forgetting” Behavior DOI Open Access
Bowen Shi,

Feiyu Ren,

Zheng Zhang

и другие.

Small, Год журнала: 2025, Номер unknown

Опубликована: Март 7, 2025

Taking inspiration from the dynamic memory of human brain, which has ability to spontaneously forget unimportant information, a universal and straightforward method for creating spatiotemporally regulated hydrogels with electrofluorochromic characteristics that exhibit information "memorizing-forgetting" behavior is presented. The reversible electrofluorochromism blue red in Eu3+-based achieved by rapid changes fluorescence triggered electricity, coupled gradual disappearance associated mass diffusion hydrogel. This process involves generation H2 an acidic aqueous solution under resulting conversion β-diketone derivatives keto enol forms disruption hydrogen bonds between ─COOH polyacrylic acid (PAA) N pyridine groups. fluorescent mechanical are facilely tuned power on time, contents components, types network structures as well derivatives. Finally, hydrogel arrays or films can be utilized programmable accurate encryption, decryption, self-erasure.

Язык: Английский

Процитировано

0
Time‐Encoded Information Encryption with pH Clock Guided Broad‐Spectrum Emission by Dynamic Assemblies DOI
Debapratim Das,

Priyam Das,

Tanushree Das

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Авг. 22, 2024

With growing threats from counterfeiting-based security breaches, multi-level and specific stimuli-responsive anti-counterfeiting devices message encryption methods have attracted immense research interest. Fluorescence-based aggregation-induced emission (AIE)-based materials solves the problems to a considerable extent. However, development of smarter patterns with hierarchical levels alongside dynamic display is still challenging. To screen out this complication, we bring forward pH-switchable fluorescent assembly an AIEgen aliphatic acid. We later temporally direct molecular aid chemical trigger-regulated pH clock, generating transitory multicolor emission, including transient white light generation. The pH-dependent emissions were further implemented in constructing smart multi-input AND gates. Subsequently, integrate time-gated emissive system develop advanced multi-dimensionally secure data strategy. This novel approach enhances measures by introducing additional layer based on temporal characteristics.

Язык: Английский

Процитировано

2
Time‐Encoded Information Encryption with pH Clock Guided Broad‐Spectrum Emission by Dynamic Assemblies DOI
Debapratim Das,

Priyam Das,

Tanushree Das

и другие.

Angewandte Chemie, Год журнала: 2024, Номер unknown

Опубликована: Авг. 22, 2024

Abstract With growing threats from counterfeiting‐based security breaches, multi‐level and specific stimuli‐responsive anti‐counterfeiting devices message encryption methods have attracted immense research interest. Fluorescence‐based aggregation‐induced emission (AIE)‐based materials solves the problems to a considerable extent. However, development of smarter patterns with hierarchical levels alongside dynamic display is still challenging. To screen out this complication, we bring forward pH‐switchable fluorescent assembly an AIEgen aliphatic acid. We later temporally direct molecular aid chemical trigger‐regulated pH clock, generating transitory multicolor emission, including transient white light generation. The pH‐dependent emissions were further implemented in constructing smart multi‐input AND gates. Subsequently, integrate time‐gated emissive system develop advanced multi‐dimensionally secure data strategy. This novel approach enhances measures by introducing additional layer based on temporal characteristics.

Язык: Английский

Процитировано

2
Boosting Microfluidic Enzymatic Cascade Reactions with pH‐Responsive Polymersomes by Spatio–Chemical Activity Control DOI Creative Commons

Andrea Koball,

Franziska Obst, Jens Gaitzsch

и другие.

Small Methods, Год журнала: 2024, Номер unknown

Опубликована: Июль 11, 2024

Abstract Microfluidic flow reactors permit the implementation of sensitive biocatalysts in polymeric environments (e.g., hydrogel dots), mimicking nature through use diverse microstructures within defined confinements. However, establishing complex hybrid structures to mimic biological processes and functions under continuous with optimal utilization all components involved reaction process represents a significant scientific challenge. To achieve spatial, chemical, temporal control for any microfluidic application, compartmentalization is required, as well unification different compartments chamber design. This study presents self‐regulating system fabricated by sequential photostructuring an intermediate chemical step realize pH‐sensitive fabrication double reactor controlled enzymatic cascade (ECR). The key point adaptation retention function pH‐responsive horseradish peroxidase‐loaded polymersomes chip flow. ECR successfully triggered interplay between glucose oxidase‐converted glucose, membrane state polymersomes, other parameters rate fluid composition). establishes promising noninvasive regulatory platform extended spatio–chemical current future systems.

Язык: Английский

Процитировано

1