Phase Transitions in Chemically Fueled, Multiphase Complex Coacervate Droplets DOI Creative Commons

Carsten Donau,

Fabian Späth, Michele Stasi

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(46)

Published: Sept. 6, 2022

Abstract Membraneless organelles are droplets in the cytosol that regulated by chemical reactions. Increasing studies suggest they internally organized. However, how these subcompartments remains elusive. Herein, we describe a complex coacervate‐based model composed of two polyanions and short peptide. With reaction cycle, control affinity peptide for polyelectrolytes leading to distinct regimes inside phase diagram. We study transitions from one regime another identify new can only occur under kinetic control. Finally, show cycle controls liquidity offering insights into active processes cells play an important role tuning liquid state membraneless organelles. Our work demonstrates not thermodynamic properties but also kinetics should be considered organization multiple phases droplets.

Language: Английский

Coacervate Droplets for Synthetic Cells DOI Creative Commons

Zi Lin,

Thomas Beneyton, Jean‐Christophe Baret

et al.

Small Methods, Journal Year: 2023, Volume and Issue: 7(12)

Published: July 18, 2023

Abstract The design and construction of synthetic cells – human‐made microcompartments that mimic features living have experienced a real boom in the past decade. While many efforts been geared toward assembling membrane‐bounded compartments, coacervate droplets produced by liquid–liquid phase separation emerged as an alternative membrane‐free compartmentalization paradigm. Here, dual role cell research is discussed: encapsulated within membrane‐enclosed coacervates act surrogates membraneless organelles ubiquitously found cells; alternatively, they can be viewed crowded cytosol‐like chassis for constructing integrated cells. After introducing key concepts coacervation illustrating chemical diversity systems, their physicochemical properties resulting bioinspired functions are emphasized. Moving from suspensions free floating coacervates, two nascent roles these highlighted: organelle‐like modules templates. Building discussion on recent studies literature, potential to assemble capable multiple life‐inspired showcased. Future challenges still tackled field finally discussed.

Language: Английский

Citations

49
Superstructural ordering in self-sorting coacervate-based protocell networks DOI
Wenjing Mu, Liyan Jia, Musen Zhou

et al.

Nature Chemistry, Journal Year: 2023, Volume and Issue: 16(2), P. 158 - 167

Published: Nov. 6, 2023

Language: Английский

Citations

45
DNA as a universal chemical substrate for computing and data storage DOI
Shuo Yang, Bas W. A. Bögels, Fei Wang

et al.

Nature Reviews Chemistry, Journal Year: 2024, Volume and Issue: 8(3), P. 179 - 194

Published: Feb. 9, 2024

Language: Английский

Citations

38
Molecular Crowding: The History and Development of a Scientific Paradigm DOI Creative Commons
Caterina Alfano, Yann Fichou, Klaus Huber

et al.

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(6), P. 3186 - 3219

Published: March 11, 2024

It is now generally accepted that macromolecules do not act in isolation but "live" a crowded environment, is, an environment populated by numerous different molecules. The field of molecular crowding has its origins the far 80s became only end 90s. In present issue, we discuss various aspects are influenced and need to consider effects. This Review meant as introduction theme analysis evolution concept through time from colloidal polymer physics more biological perspective. We introduce themes will be thoroughly treated other Reviews issue. our intentions, each may stand itself, complete collection aspiration provide complementary perspectives propose holistic view crowding.

Language: Английский

Citations

37
The role of biomolecular condensates in protein aggregation DOI
Brent S. Visser, Wojciech P. Lipiński, Evan Spruijt

et al.

Nature Reviews Chemistry, Journal Year: 2024, Volume and Issue: 8(9), P. 686 - 700

Published: Aug. 12, 2024

Language: Английский

Citations

23
Tuning the viscoelastic properties of peptide coacervates by single amino acid mutations and salt kosmotropicity DOI Creative Commons

Xi Wu,

Yue Sun, Jing Yu

et al.

Communications Chemistry, Journal Year: 2024, Volume and Issue: 7(1)

Published: Jan. 4, 2024

Abstract Coacervation, or liquid-liquid phase separation (LLPS) of biomacromolecules, is increasingly recognized to play an important role both intracellularly and in the extracellular space. Central questions that remain be addressed are links between material properties coacervates (condensates) primary secondary structures their constitutive building blocks. Short LLPS-prone peptides, such as GY23 variants explored this study, ideal model systems investigate these because simple sequence modifications chemical environment strongly affect viscoelastic coacervates. Herein, a systematic investigation structure/property relationships peptide was conducted using variants, combining biophysical characterization (plate rheology surface force apparatus, SFA) with structure investigations by infrared (IR) circular dichroism (CD) spectroscopy. Mutating specific residues into either more hydrophobic hydrophilic regulates Furthermore, ionic strength kosmotropic characteristics (Hofmeister series) buffer which LLPS induced also significantly impact formed Structural CD IR indicate direct correlation variations endogenous (peptide sequence) exogenous (ionic strength, characteristics, aging) factors β-sheet content within These findings provide valuable insights rationally design short programmable materials used biomedical applications.

Language: Английский

Citations

20
Self-assembly of stabilized droplets from liquid–liquid phase separation for higher-order structures and functions DOI Creative Commons
Mehwish Naz,

Lin Zhang,

Chong Chen

et al.

Communications Chemistry, Journal Year: 2024, Volume and Issue: 7(1)

Published: April 9, 2024

Dynamic microscale droplets produced by liquid-liquid phase separation (LLPS) have emerged as appealing biomaterials due to their remarkable features. However, the instability of limits construction population-level structures with collective behaviors. Here we first provide a brief background in context materials properties. Subsequently, discuss current strategies for stabilizing including physical and chemical modulation. We also recent development LLPS various applications such synthetic cells biomedical materials. Finally, give insights on how stabilized can self-assemble into higher-order displaying coordinated functions fully exploit potentials bottom-up biology applications.

Language: Английский

Citations

17
Molecular Design of Chemically Fueled Peptide–Polyelectrolyte Coacervate-Based Assemblies DOI
Fabian Späth,

Carsten Donau,

Alexander M. Bergmann

et al.

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 143(12), P. 4782 - 4789

Published: March 22, 2021

Complex coacervated-based assemblies form when two oppositely charged polyelectrolytes combine to phase separate into a supramolecular architecture. These architectures range from complex coacervate droplets, spherical and worm-like micelles, vesicles. are widely applied, for example, in the food industry, as underwater or medical adhesives, but they can also serve great model biological assemblies. Indeed, biology relies on coacervation so-called membraneless organelles, dynamic transient droplets formed by of nucleic acids proteins. To regulate their function, organelles dynamically maintained chemical reaction cycles, including phosphorylation dephosphorylation, exact mechanisms remain elusive. Recently, some systems regulated cycles have been introduced, how design such molecular affects properties is unclear. In this work, we test series cationic peptides chemically fueled coacervation, affect dynamics assembly disassembly emerging structures. We them with both homo- block copolymers study morphologies assemblies, morphological transitions that driven cycle. deduce heuristic rules be applied other systems. will help develop organelle lead exciting new applications coacervate-based examples like temporary adhesives.

Language: Английский

Citations

98
Driving force and pathway in polyelectrolyte complex coacervation DOI Creative Commons
Shensheng Chen, Zhen‐Gang Wang

Proceedings of the National Academy of Sciences, Journal Year: 2022, Volume and Issue: 119(36)

Published: Aug. 29, 2022

There is notable discrepancy between experiments and coarse-grained model studies regarding the thermodynamic driving force in polyelectrolyte complex coacervation: find free energy change to be dominated by entropy, while simulations using models with implicit solvent usually report a large, even dominant energetic contribution systems weak intermediate electrostatic strength. Here, coarse-grained, implicit-solvent molecular dynamics simulation combined analysis, we study potential of mean (PMF) two key stages on coacervation pathway for symmetric mixtures: polycation–polyanion complexation polyion pair–pair condensation. We show that temperature dependence dielectric constant water gives rise substantial entropic interaction. By accounting this which due reorganization, under common conditions (monovalent ions, room temperature) aqueous systems, both are strongly entropy-driven negligible or unfavorable contributions, consistent experimental results. Furthermore, strengths, rather than counterion-release primary entropy contribution. From calculated PMF, supernatant phase consists predominantly pairs vanishingly small concentration bare polyelectrolytes, provide an estimate spinodal phase. Finally, prior contact, neutral weakly attract each other mutually induced polarization, providing initial fusion pairs.

Language: Английский

Citations

64
Triggerable Protocell Capture in Nanoparticle-Caged Coacervate Microdroplets DOI Creative Commons
Ning Gao,

Can Xu,

Zhuping Yin

et al.

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(9), P. 3855 - 3862

Published: Feb. 22, 2022

Controlling the dynamics of mixed communities cell-like entities (protocells) provides a step toward development higher-order cytomimetic behaviors in artificial cell consortia. In this paper, we develop caged protocell model with molecularly crowded coacervate interior surrounded by non-cross-linked gold (Au)/poly(ethylene glycol) (PEG) nanoparticle-jammed stimuli-responsive membrane. The jammed membrane is unlocked either exogenous light-mediated Au/PEG dissociation at Au surface or endogenous enzyme-mediated cleavage ketal linkage on PEG backbone. assembly/disassembly process used for controlled and selective uptake guest protocells into microdroplets as path an all-water triggerable transmembrane synthetic communities. Active capture stems from high sequestration potential such that tailoring properties rudimentary system sorting. Our results highlight programming surface-contact interactions between membrane-bounded compartments could have implications networks, storage delivery microsystems, microreactor technologies.

Language: Английский

Citations

63