Abstract The spontaneous assembly of chemically encoded, molecularly crowded, water-rich micro-droplets into periodic defect-free two-dimensional arrays is achieved in aqueous media by a combination an acoustic standing wave pressure field and situ complex coacervation. Acoustically mediated coalescence primary droplets generates single-droplet per node micro-arrays that exhibit variable surface-attachment properties, spontaneously uptake dyes, enzymes particles, display spatial...

Abstract Coacervate microdroplets produced by liquid–liquid phase separation have been used as synthetic protocells that mimic the dynamical organization of membrane‐free organelles in living systems. Achieving spatiotemporal control over droplet condensation and disassembly remains challenging. Herein, we describe formation photoswitchable behavior light‐responsive coacervate droplets prepared from mixtures double‐stranded DNA an azobenzene cation. The disassemble reassemble under UV blue...

Abstract Fabrication of compartmentalised chemical systems with nested architectures and biomimetic properties has important implications for controlling the positional assembly functional components, spatiotemporal regulation enzyme cascades modelling proto-organelle behaviour in synthetic protocells. Here, we describe spontaneous capture glucose oxidase-containing proteinosomes pH-sensitive fatty acid micelle coacervate droplets as a facile route to multi-compartmentalised host–guest...

Intrinsic differences in the molecular sequestration of folded and unfolded proteins within poly(diallyldimethylammonium) (PDDA)/poly(acrylate) (PAA) coacervate microdroplets are exploited to establish membrane-free microcompartments that support protein refolding, facilitate recovery secondary structure enzyme activity, enable selective uptake exclusion biomolecules, respectively. Native bovine serum albumin, carbonic anhydrase, α-chymotrypsin preferentially sequestered positively charged...

Abstract Modern cells are complex chemical compartments tightly regulated by an underlying DNA-encoded program. Achieving a form of coupling between molecular content, reactions, and chassis in synthetic represents key step to the assembly evolvable protocells but remains challenging. Here, we design coacervate droplets that promote non-enzymatic oligonucleotide polymerization restructure as result reaction dynamics. More specifically, rationally exploit complexation end-reactive...

Abstract We report on the formation of surfactant‐based complex catanionic coacervate droplets in mixtures decanoic acid and cetylpyridinium chloride or cetyltrimethylammonium bromide. show that coacervation occurs over a broad range composition, pH, ionic strength. The coacervates consist elongated micelles, sequester wide solutes including water‐soluble organic dyes, polysaccharides, proteins, enzymes, DNA, can be structurally stabilized by sodium alginate gelatin‐based hydrogelation....

Abstract The fabrication of stable colloidosomes derived from water‐in‐water Pickering‐like emulsions are described that were produced by addition fluorescent amine‐modified polystyrene latex beads to an aqueous two‐phase system consisting dextran‐enriched droplets dispersed in a PEG‐enriched continuous phase. Addition polyacrylic acid followed carbodiimide‐induced crosslinking with dextran produces hydrogelled capable reversible swelling and selective molecular uptake exclusion....

Membraneless organelles are phase-separated droplets that dynamically assembled and dissolved in response to biochemical reactions cells. Complex coacervate produced by associative liquid-liquid phase separation offer a promising approach mimic such dynamic compartmentalization. Here, we present model for membraneless based on enzyme/polyelectrolyte complex coacervates able induce their own condensation dissolution. We show glucose oxidase forms with cationic polysaccharide narrow pH range,...

Abstract The prebiotic organization of chemicals into compartmentalized ensembles is an essential step to understand the transition from inert molecules living matter. Compartmentalization indeed a central property systems. Fatty acids represent simplest amphiphiles capable self‐assembling membrane‐bound vesicles, and have therefore emerged as valuable create models protocellular compartments. Here, main experimental findings supporting this idea are reviewed, together with approaches...

Abstract Biomolecular condensates are membraneless organelles that orchestrate various metabolic pathways in living cells. Understanding how these crowded structures regulate enzyme reactions remains yet challenging due to their dynamic and intricate nature. Coacervate microdroplets formed by associative liquid‐liquid phase separation of oppositely charged polyions have emerged as relevant condensate models study catalysis. Enzyme within droplets show altered kinetics, influenced factors...

Multiphase coacervate droplets produced by internalised aqueous two-phase separation are used for the spatially dependent chemical transfer of sugar molecules.

Abstract Coacervate microdroplets produced by liquid–liquid phase separation have been used as synthetic protocells that mimic the dynamical organization of membrane‐free organelles in living systems. Achieving spatiotemporal control over droplet condensation and disassembly remains challenging. Herein, we describe formation photoswitchable behavior light‐responsive coacervate droplets prepared from mixtures double‐stranded DNA an azobenzene cation. The disassemble reassemble under UV blue...

Complex coacervate microdroplets, which are formed via spontaneous liquid-liquid phase separation by mixing two oppositely charged polyelectrolytes in water, have emerged as a new paradigm the fields of origin life, membraneless subcellular compartmentalization, bioreactors, and drug delivery. However, how to further improve its stability enhance selectivity one particular system remains challenge. By generating membrane-like layer at surface microdroplets electrostatic interactions between...

Prevention of thermal aggregation antibodies in aqueous solutions was achieved by noncovalent association with hydrophobically modified poly(acrylate) copolymers. Using a polyclonal immunoglobin G (IgG) as model system for antibodies, we have studied the mechanisms which this multidomain protein interacts polyanions when incubated at physiological pH and temperatures below above unfolding/denaturation temperature, salt-free 0.1 M NaCl solutions. The selected were sodium poly(acrylates),...

Light-induced shape transformations represent a fundamental step towards the emergence of adaptive materials exhibiting photomechanical behaviours. Although range covalent azobenzene-based photoactive has been demonstrated, use dynamic photoisomerization in mesostructured soft solids involving non-covalent co-assembly received little attention. Here we prepare discrete micrometre-sized hydrated particles hexagonally ordered polyelectrolyte-surfactant mesophase based on electrostatically...

Coupling a hydrophobic drug onto monoclonal antibodies via lysine residues is common route to prepare antibody–drug conjugates (ADC), promising class of biotherapeutics. But few chemical modifications on protein surface often increase aggregation propensity, without clear understanding the mechanisms at stake (loss colloidal stability, self-assemblies, denaturation, etc.), and statistical nature conjugation introduces polydispersity in ADC population, which raises questions whether whole...

Abstract Advancing the spontaneous bottom-up construction of artificial cells with high organisational complexity and diverse functionality remains an unresolved issue at interface between living non-living matter. To address this challenge, a material assembly process based on capture on-site processing spatially segregated bacterial colonies within individual coacervate micro-droplets is developed for endogenous membrane-bounded, molecularly crowded, compositionally, structurally...