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Journal articles on the topic 'Dynamic coacervates'

Author: Grafiati

Published: 26 October 2024

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1

Furlani, Franco, Pietro Parisse, and Pasquale Sacco. "On the Formation and Stability of Chitosan/Hyaluronan-Based Complex Coacervates." Molecules 25, no. 5 (February 27, 2020): 1071. http://dx.doi.org/10.3390/molecules25051071.

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This contribution is aimed at extending our previous findings on the formation and stability of chitosan/hyaluronan-based complex coacervates. Colloids are herewith formed by harnessing electrostatic interactions between the two polyelectrolytes. The presence of tiny amounts of the multivalent anion tripolyphosphate (TPP) in the protocol synthesis serves as an adjuvant “point-like” cross-linker for chitosan. Hydrochloride chitosans at different viscosity average molar mass, M v ¯ , in the range 10,000–400,000 g/mol, and fraction of acetylated units, FA, (0.16, 0.46 and 0.63) were selected to fabricate a large library of formulations. Concepts such as coacervate size, surface charge and homogeneity in relation to chitosan variables are herein disclosed. The stability of coacervates in Phosphate Buffered Saline (PBS) was verified by means of scattering techniques, i.e., Dynamic Light Scattering (DLS) and Small-Angle X-ray Scattering (SAXS). The conclusions from this set of experiments are the following: (i) a subtle equilibrium between chitosan FA and M v ¯ does exist in ensuring colloidal stability; (ii) once diluted in PBS, osmotic swelling-driven forces trigger the enlargement of the polymeric mesh with an ensuing increase of coacervate size and porosity.

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2

Zheng, Jiabao, Qing Gao, Ge Ge, Jihong Wu, Chuan-he Tang, Mouming Zhao, and Weizheng Sun. "Dynamic equilibrium of β-conglycinin/lysozyme heteroprotein complex coacervates." Food Hydrocolloids 124 (March 2022): 107339. http://dx.doi.org/10.1016/j.foodhyd.2021.107339.

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3

Vecchies, Federica, Pasquale Sacco, Eleonora Marsich, Giuseppe Cinelli, Francesco Lopez, and Ivan Donati. "Binary Solutions of Hyaluronan and Lactose-Modified Chitosan: The Influence of Experimental Variables in Assembling Complex Coacervates." Polymers 12, no. 4 (April 13, 2020): 897. http://dx.doi.org/10.3390/polym12040897.

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A miscibility study between oppositely charged polyelectrolytes, namely hyaluronic acid and a lactose-modified chitosan, is here reported. Experimental variables such as polymers’ weight ratios, pH values, ionic strengths and hyaluronic acid molecular weights were considered. Transmittance analyses demonstrated the mutual solubility of the two biopolymers at a neutral pH. The onset of the liquid-liquid phase separation due to electrostatic interactions between the two polymers was detected at pH 4.5, and it was found to be affected by the overall ionic strength, the modality of mixing and the polymers’ weight ratio. Thorough Dynamic Light Scattering (DLS) measurements were performed to check the quality of the formed coacervates by investigating their dimensions, homogeneity and surface charge. The whole DLS results highlighted the influence of the hyaluronic acid molecular weight in affecting coacervates’ dispersity and size.

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4

Aponte-Rivera, Christian, and Michael Rubinstein. "Dynamic Coupling in Unentangled Liquid Coacervates Formed by Oppositely Charged Polyelectrolytes." Macromolecules 54, no. 4 (January 29, 2021): 1783–800. http://dx.doi.org/10.1021/acs.macromol.0c01393.

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5

Mohanty, B., V. K. Aswal, P. S. Goyal, and H. B. Bohidar. "Small-angle neutron and dynamic light scattering study of gelatin coacervates." Pramana 63, no. 2 (August 2004): 271–76. http://dx.doi.org/10.1007/bf02704984.

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6

Lin, Ya’nan, Hairong Jing, Zhijun Liu, Jiaxin Chen, and Dehai Liang. "Dynamic Behavior of Complex Coacervates with Internal Lipid Vesicles under Nonequilibrium Conditions." Langmuir 36, no. 7 (January 31, 2020): 1709–17. http://dx.doi.org/10.1021/acs.langmuir.9b03561.

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7

Wang, Lechuan, Mengzhuo Liu, Panpan Guo, Huajiang Zhang, Longwei Jiang, Ning Xia, Li Zheng, Qian Cui, and Shihui Hua. "Understanding the structure, interfacial properties, and digestion fate of high internal phase Pickering emulsions stabilized by food-grade coacervates: Tracing the dynamic transition from coacervates to complexes." Food Chemistry 414 (July 2023): 135718. http://dx.doi.org/10.1016/j.foodchem.2023.135718.

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8

Furlani, Franco, Ivan Donati, Eleonora Marsich, and Pasquale Sacco. "Characterization of Chitosan/Hyaluronan Complex Coacervates Assembled by Varying Polymers Weight Ratio and Chitosan Physical-Chemical Composition." Colloids and Interfaces 4, no. 1 (March 2, 2020): 12. http://dx.doi.org/10.3390/colloids4010012.

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Herein, we synthetized and characterized polysaccharide-based complex coacervates starting from two water-soluble biopolymers, i.e., hydrochloride chitosans and sodium hyaluronan. We used chitosans encompassing a range of molecular weights from 30,000 to 400,000 and showing different fraction of acetylated units (i.e., FA = 0.16, 0.46, and 0.63). This set of chitosans was mixed with a low molecular weight hyaluronan to promote electrostatic interactions. Resulting colloids were analyzed in terms of size, polydispersity and surface charge by Dynamic Light Scattering. The weight ratio between the two polyelectrolytes was studied as additional parameter influencing the liquid-liquid phase separation. Main results include the following: the polymers weight ratio was fundamental in dictating the colloids surface charge, whereas chitosan physical-chemical features influenced the dimension and homogeneity of colloids. This contribution presents additional understanding of the complex coacervation between these two oppositely charged polysaccharides, with the potential translation of present system in food and biomedical sectors.

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9

Bohidar, H., P. L. Dubin, P. R. Majhi, C. Tribet, and W. Jaeger. "Effects of Protein−Polyelectrolyte Affinity and Polyelectrolyte Molecular Weight on Dynamic Properties of Bovine Serum Albumin−Poly(diallyldimethylammonium chloride) Coacervates." Biomacromolecules 6, no. 3 (May 2005): 1573–85. http://dx.doi.org/10.1021/bm049174p.

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10

Danielsen, Scott P. O., James McCarty, Joan-Emma Shea, Kris T. Delaney, and Glenn H. Fredrickson. "Molecular design of self-coacervation phenomena in block polyampholytes." Proceedings of the National Academy of Sciences 116, no. 17 (April 4, 2019): 8224–32. http://dx.doi.org/10.1073/pnas.1900435116.

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Coacervation is a common phenomenon in natural polymers and has been applied to synthetic materials systems for coatings, adhesives, and encapsulants. Single-component coacervates are formed when block polyampholytes exhibit self-coacervation, phase separating into a dense liquid coacervate phase rich in the polyampholyte coexisting with a dilute supernatant phase, a process implicated in the liquid–liquid phase separation of intrinsically disordered proteins. Using fully fluctuating field-theoretic simulations using complex Langevin sampling and complementary molecular-dynamics simulations, we develop molecular design principles to connect the sequenced charge pattern of a polyampholyte with its self-coacervation behavior in solution. In particular, the lengthscale of charged blocks and number of connections between oppositely charged blocks are shown to have a dramatic effect on the tendency to phase separate and on the accessible chain conformations. The field and particle-based simulation results are compared with analytical predictions from the random phase approximation (RPA) and postulated scaling relationships. The qualitative trends are mostly captured by the RPA, but the approximation fails catastrophically at low concentration.

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11

Bos, Inge, Eline Brink, Lucile Michels, and Joris Sprakel. "DNA dynamics in complex coacervate droplets and micelles." Soft Matter 18, no. 10 (2022): 2012–27. http://dx.doi.org/10.1039/d1sm01787j.

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DNA can be mixed with oppositely charged homopolymers or diblock copolymers to form respectively complex coacervate droplets or complex coacervate core micelles. We study the chain length effect on the dynamics of these complex coacervate structures.

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12

Tom, Jenna K. A., and Ashok A. Deniz. "Complex dynamics of multicomponent biological coacervates." Current Opinion in Colloid & Interface Science 56 (December 2021): 101488. http://dx.doi.org/10.1016/j.cocis.2021.101488.

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13

Peixoto, Paulo D. S., Guilherme M. Tavares, Thomas Croguennec, Aurélie Nicolas, Pascaline Hamon, Claire Roiland, and Saïd Bouhallab. "Structure and Dynamics of Heteroprotein Coacervates." Langmuir 32, no. 31 (July 26, 2016): 7821–28. http://dx.doi.org/10.1021/acs.langmuir.6b01015.

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14

Wang, Shengbo, Changlong Chen, Bor-Jier Shiau, and Jeffrey H. Harwell. "Counterion binding on coacervation of dioctyl sulfosuccinate in aqueous sodium chloride." Soft Matter 15, no. 18 (2019): 3771–78. http://dx.doi.org/10.1039/c8sm02531b.

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A simple coacervate-forming system consisting of sodium dioctyl sulfosuccinate (DOSS) in aqueous NaCl solution was investigated by turbidity measurement, electromotive force measurement (EMF), dynamic light scattering (DLS), and cryogenic transmission electron microscopy (cryo-TEM) to reveal the role of counterion binding in the microstructural changes behind the evolution of the coacervate phase.

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15

Kausik, Ravinath, Aasheesh Srivastava, Peter A. Korevaar, Galen Stucky, J. Herbert Waite, and Songi Han. "Local Water Dynamics in Coacervated Polyelectrolytes Monitored through Dynamic Nuclear Polarization-Enhanced1H NMR." Macromolecules 42, no. 19 (October 13, 2009): 7404–12. http://dx.doi.org/10.1021/ma901137g.

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16

Kausik, Ravinath, Aasheesh Srivastava, Peter A. Korevaar, Galen Stucky, J. Herbert Waite, and Songi Han. "Local Water Dynamics in Coacervated Polyelectrolytes Monitored through Dynamic Nuclear Polarization-Enhanced1H NMR." Macromolecules 43, no. 6 (March 23, 2010): 3122. http://dx.doi.org/10.1021/ma902825f.

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17

Armstrong, James P. K., Sam N. Olof, Monika D. Jakimowicz, Anthony P. Hollander, Stephen Mann, Sean A. Davis, Mervyn J. Miles, Avinash J. Patil, and Adam W. Perriman. "Cell paintballing using optically targeted coacervate microdroplets." Chemical Science 6, no. 11 (2015): 6106–11. http://dx.doi.org/10.1039/c5sc02266e.

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18

Karoui, Hedi, Marianne J. Seck, and Nicolas Martin. "Self-programmed enzyme phase separation and multiphase coacervate droplet organization." Chemical Science 12, no. 8 (2021): 2794–802. http://dx.doi.org/10.1039/d0sc06418a.

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19

Lambden, Edward, and Martin B. Ulmschneider. "Coarse grained antimicrobial coacervated nanoparticle dynamics." Biophysical Journal 122, no. 3 (February 2023): 371a. http://dx.doi.org/10.1016/j.bpj.2022.11.2044.

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20

Kayitmazer, A. Basak, Himadri B. Bohidar, Kevin W. Mattison, Arijit Bose, Jayashri Sarkar, Akihito Hashidzume, Paul S. Russo, Werner Jaeger, and Paul L. Dubin. "Mesophase separation and probe dynamics in protein–polyelectrolyte coacervates." Soft Matter 3, no. 8 (2007): 1064–76. http://dx.doi.org/10.1039/b701334e.

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21

Yu, Boyuan, Phillip M. Rauscher, Nicholas E. Jackson, Artem M. Rumyantsev, and Juan J. de Pablo. "Crossover from Rouse to Reptation Dynamics in Salt-Free Polyelectrolyte Complex Coacervates." ACS Macro Letters 9, no. 9 (August 26, 2020): 1318–24. http://dx.doi.org/10.1021/acsmacrolett.0c00522.

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22

Fighir, Daniela, Carmen Paduraru, Ramona Ciobanu, Florin Bucatariu, Oana Plavan, Andreea Gherghel, George Barjoveanu, Marcela Mihai, and Carmen Teodosiu. "Removal of Diclofenac and Heavy Metal Ions from Aqueous Media Using Composite Sorbents in Dynamic Conditions." Nanomaterials 14, no. 1 (December 21, 2023): 33. http://dx.doi.org/10.3390/nano14010033.

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Pharmaceuticals and heavy metals pose significant risks to human health and aquatic ecosystems, necessitating their removal from water and wastewater. A promising alternative for this purpose involves their removal by adsorption on composite sorbents prepared using a conventional layer-by-layer (LbL) method or an innovative coacervate direct deposition approach. In this study, four novel composite materials based on a silica core (IS) and a polyelectrolyte coacervate shell were used for the investigation of dynamic adsorption of three heavy metals (lead, nickel and cadmium) and an organic drug model (diclofenac sodium salt, DCF-Na). The four types of composite sorbents were tested for the first time in dynamic conditions (columns with continuous flow), and the column conditions were similar to those used in wastewater treatment plants. The influence of the polyanion nature (poly(acrylic acid) (PAA) vs. poly(sodium methacrylate) (PMAA)), maintaining a constant poly(ethyleneimine) (PEI), and the cross-linking degree (r = 0.1 and r = 1.0) of PEI chains on the immobilization of these pollutants (inorganic vs. organic) on the same type of composite was also studied. The experiments involved both single- and multi-component aqueous solutions. The kinetics of the dynamic adsorption process were examined using two non-linear models: the Thomas and Yoon–Nelson models. The tested sorbents demonstrated good adsorption capacities with affinities for the metal ions in the following order: Pb2+ > Cd2+ > Ni2+. An increase in the initial diclofenac sodium concentration led to an enhanced adsorption capacity of the IS/(PEI-PAA)c-r1 sorbent. The calculated sorption capacities were in good agreement with the adsorption capacity predicted by the Thomas and Yoon–Nelson models. The substantial affinity observed between DCF-Na and a column containing composite microparticles saturated with heavy metal ions was explained.

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23

Ortony, Julia H., Dong Soo Hwang, John M. Franck, J. Herbert Waite, and Songi Han. "Asymmetric Collapse in Biomimetic Complex Coacervates Revealed by Local Polymer and Water Dynamics." Biomacromolecules 14, no. 5 (April 19, 2013): 1395–402. http://dx.doi.org/10.1021/bm4000579.

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24

Reichheld, Sean E., Lisa D. Muiznieks, Fred W. Keeley, and Simon Sharpe. "Direct observation of structure and dynamics during phase separation of an elastomeric protein." Proceedings of the National Academy of Sciences 114, no. 22 (May 15, 2017): E4408—E4415. http://dx.doi.org/10.1073/pnas.1701877114.

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Despite its growing importance in biology and in biomaterials development, liquid–liquid phase separation of proteins remains poorly understood. In particular, the molecular mechanisms underlying simple coacervation of proteins, such as the extracellular matrix protein elastin, have not been reported. Coacervation of the elastin monomer, tropoelastin, in response to heat and salt is a critical step in the assembly of elastic fibers in vivo, preceding chemical cross-linking. Elastin-like polypeptides (ELPs) derived from the tropoelastin sequence have been shown to undergo a similar phase separation, allowing formation of biomaterials that closely mimic the material properties of native elastin. We have used NMR spectroscopy to obtain site-specific structure and dynamics of a self-assembling elastin-like polypeptide along its entire self-assembly pathway, from monomer through coacervation and into a cross-linked elastic material. Our data reveal that elastin-like hydrophobic domains are composed of transient β-turns in a highly dynamic and disordered chain, and that this disorder is retained both after phase separation and in elastic materials. Cross-linking domains are also highly disordered in monomeric and coacervated ELP3 and form stable helices only after chemical cross-linking. Detailed structural analysis combined with dynamic measurements from NMR relaxation and diffusion data provides direct evidence for an entropy-driven mechanism of simple coacervation of a protein in which transient and nonspecific intermolecular hydrophobic contacts are formed by disordered chains, whereas bulk water and salt are excluded.

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25

Arfin, Najmul, Avinash Chand Yadav, and H. B. Bohidar. "Sub-diffusion and trapped dynamics of neutral and charged probes in DNA-protein coacervates." AIP Advances 3, no. 11 (November 2013): 112108. http://dx.doi.org/10.1063/1.4830281.

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26

Wee, Wen Ann, Hiroshi Sugiyama, and Soyoung Park. "Photoswitchable single-stranded DNA-peptide coacervate formation as a dynamic system for reaction control." iScience 24, no. 12 (December 2021): 103455. http://dx.doi.org/10.1016/j.isci.2021.103455.

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27

Kim, Jung-Min, Tae-Young Heo, and Soo-Hyung Choi. "Structure and Relaxation Dynamics for Complex Coacervate Hydrogels Formed by ABA Triblock Copolymers." Macromolecules 53, no. 21 (October 1, 2020): 9234–43. http://dx.doi.org/10.1021/acs.macromol.0c01600.

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28

Amali, Arlin Jose, Shashi Singh, Nandini Rangaraj, Digambara Patra, and Rohit Kumar Rana. "Poly(l-Lysine)–pyranine-3 coacervate mediated nanoparticle-assembly: fabrication of dynamic pH-responsive containers." Chem. Commun. 48, no. 6 (2012): 856–58. http://dx.doi.org/10.1039/c1cc15209b.

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29

Li, Nan K., Yuxin Xie, and Yaroslava G. Yingling. "Insights into Structure and Aggregation Behavior of Elastin-like Polypeptide Coacervates: All-Atom Molecular Dynamics Simulations." Journal of Physical Chemistry B 125, no. 30 (July 21, 2021): 8627–35. http://dx.doi.org/10.1021/acs.jpcb.1c02822.

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30

Spruijt, Evan, Frans A. M. Leermakers, Remco Fokkink, Ralf Schweins, Ad A. van Well, Martien A. Cohen Stuart, and Jasper van der Gucht. "Structure and Dynamics of Polyelectrolyte Complex Coacervates Studied by Scattering of Neutrons, X-rays, and Light." Macromolecules 46, no. 11 (May 31, 2013): 4596–605. http://dx.doi.org/10.1021/ma400132s.

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31

Lappan, Uwe, Brigitte Wiesner, and Ulrich Scheler. "Segmental Dynamics of Poly(acrylic acid) in Polyelectrolyte Complex Coacervates Studied by Spin-Label EPR Spectroscopy." Macromolecules 49, no. 22 (November 3, 2016): 8616–21. http://dx.doi.org/10.1021/acs.macromol.6b01863.

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32

Nolles, Antsje, Ellard Hooiveld, Adrie H. Westphal, Willem J. H. van Berkel, J. Mieke Kleijn, and Jan Willem Borst. "FRET Reveals the Formation and Exchange Dynamics of Protein-Containing Complex Coacervate Core Micelles." Langmuir 34, no. 40 (September 13, 2018): 12083–92. http://dx.doi.org/10.1021/acs.langmuir.8b01272.

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33

Gibson, Iain, Arash Momeni, and Mark Filiaggi. "Minocycline-loaded calcium polyphosphate glass microspheres as a potential drug-delivery agent for the treatment of periodontitis." Journal of Applied Biomaterials & Functional Materials 17, no. 3 (July 2019): 228080001986363. http://dx.doi.org/10.1177/2280800019863637.

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Background: Periodontitis is an inflammatory disease with a bacterial etiology that affects the supporting structures of the teeth and is a major cause of tooth loss. The objective of this study was to investigate the drug loading and in vitro release of minocycline from novel calcium polyphosphate microspheres intended for use in treating periodontitis. Methods: Calcium polyphosphate coacervate, produced by a precipitation reaction of calcium chloride and sodium polyphosphate solutions, was loaded with minocycline and subsequently used to produce microspheres by an emulsion/solvent extraction technique. Microspheres classified by size were subjected to a 7-day elution in a Tris-buffer solution under dynamic conditions. The physicochemical characteristics of the drug-loaded microspheres were investigated using scanning electron microscopy, particle size analysis, Phosphorus-31 Nuclear Magnetic Resonance spectroscopy, and Inductively Coupled Plasma Optical Emission Spectroscopy. Drug loading and release were determined using ultraviolet -visible (UV/VIS) spectrophotometry. Results: Minocycline-loaded calcium polyphosphate microspheres of varying size were successfully produced, with small and large microspheres having volume mean diameters of 22 ± 1 µm and 193 ± 5 µm, respectively. Polyphosphate chain length and calcium to phosphorus mole ratio remained stable throughout microsphere production. Drug loading was 1.64 ± 0.16, 1.35 ± 0.55, and 0.84 ± 0.14 weight% for the coacervate and large and small microspheres, respectively, corresponding to mean encapsulation efficiencies of 81.7 ± 12.2 % and 50.9 ± 3.9 % for the large and small microspheres. Sustained drug release was observed in vitro over a clinically relevant 7-day period, with small and large microspheres exhibiting similar elution profiles. Antibiotic release generally followed microsphere degradation as measured by Ca and P ion release. Conclusions: This study demonstrated successful drug loading of calcium polyphosphate microspheres with minocycline. Furthermore, in vitro sustained release of minocycline over a 7-day period was observed, suggesting potential utility of this approach for treating periodontitis.

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34

Zheng, Jiabao, Qing Gao, Ge Ge, Jihong Wu, Chuan-he Tang, Mouming Zhao, and Weizheng Sun. "Heteroprotein Complex Coacervate Based on β-Conglycinin and Lysozyme: Dynamic Protein Exchange, Thermodynamic Mechanism, and Lysozyme Activity." Journal of Agricultural and Food Chemistry 69, no. 28 (July 9, 2021): 7948–59. http://dx.doi.org/10.1021/acs.jafc.1c02204.

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35

Anvari, Mohammad, and Donghwa Chung. "Dynamic rheological and structural characterization of fish gelatin – Gum arabic coacervate gels cross-linked by tannic acid." Food Hydrocolloids 60 (October 2016): 516–24. http://dx.doi.org/10.1016/j.foodhyd.2016.04.028.

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36

Lappan, Uwe, and Ulrich Scheler. "Influence of the Nature of the Ion Pairs on the Segmental Dynamics in Polyelectrolyte Complex Coacervate Phases." Macromolecules 50, no. 21 (October 24, 2017): 8631–36. http://dx.doi.org/10.1021/acs.macromol.7b01858.

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37

Liu, Wei, Jie Deng, Siyu Song, Soumya Sethi, and Andreas Walther. "A facile DNA coacervate platform for engineering wetting, engulfment, fusion and transient behavior." Communications Chemistry 7, no. 1 (May 1, 2024). http://dx.doi.org/10.1038/s42004-024-01185-4.

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AbstractBiomolecular coacervates are emerging models to understand biological systems and important building blocks for designer applications. DNA can be used to build up programmable coacervates, but often the processes and building blocks to make those are only available to specialists. Here, we report a simple approach for the formation of dynamic, multivalency-driven coacervates using long single-stranded DNA homopolymer in combination with a series of palindromic binders to serve as a synthetic coacervate droplet. We reveal details on how the length and sequence of the multivalent binders influence coacervate formation, how to introduce switching and autonomous behavior in reaction circuits, as well as how to engineer wetting, engulfment and fusion in multi-coacervate system. Our simple-to-use model DNA coacervates enhance the understanding of coacervate dynamics, fusion, phase transition mechanisms, and wetting behavior between coacervates, forming a solid foundation for the development of innovative synthetic and programmable coacervates for fundamental studies and applications.

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38

Appelhans, Dietmar, Yang Zhou, Kehu Zhang, Silvia Moreno, Achim Temme, and Brigitte Voit. "Continuous Transformation from Membrane‐less Coacervates to Membranized Coacervates and Giant Vesicles: toward Multicompartmental Protocells with Complex (Membrane) Architectures." Angewandte Chemie, June 7, 2024. http://dx.doi.org/10.1002/ange.202407472.

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The membranization of membrane‐less coacervates paves the way for the exploitation of complex protocells with regard to structural and cell‐like functional behaviors. However, the controlled transformation from membranized coacervates to vesicles remains a challenge. This can provide stable (multi)phase and (multi)compartmental architectures through the reconfiguration of coacervate droplets in the presence of (bioactive) polymers, bio(macro)molecules and/or nanoobjects. Herein, we present a continuous protocell transformation from membrane‐less coacervates to membranized coacervates and, ultimately, to giant hybrid vesicles. This transformation process is orchestrated by altering the balance of non‐covalent interactions through varying concentrations of an anionic terpolymer, leading to dynamic processes such as spontaneous membranization of terpolymer nanoparticles at the coacervate surface, disassembly of the coacervate phase mediated by the excess anionic charge, and the redistribution of coacervate components in membrane. The diverse protocells during the transformation course provide distinct structural features and molecular permeability. Notably, the introduction of multiphase coacervates in this continuous transformation process signifies advancements toward the creation of synthetic cells with different diffusible compartments. Our findings emphasize the highly controlled continuous structural reorganization of coacervate protocells and represents a novel step toward the development of advanced and sophisticated synthetic protocells with more precise compositions and complex (membrane) structures.

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39

Appelhans, Dietmar, Yang Zhou, Kehu Zhang, Silvia Moreno, Achim Temme, and Brigitte Voit. "Continuous Transformation from Membrane‐less Coacervates to Membranized Coacervates and Giant Vesicles: toward Multicompartmental Protocells with Complex (Membrane) Architectures." Angewandte Chemie International Edition, June 7, 2024. http://dx.doi.org/10.1002/anie.202407472.

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The membranization of membrane‐less coacervates paves the way for the exploitation of complex protocells with regard to structural and cell‐like functional behaviors. However, the controlled transformation from membranized coacervates to vesicles remains a challenge. This can provide stable (multi)phase and (multi)compartmental architectures through the reconfiguration of coacervate droplets in the presence of (bioactive) polymers, bio(macro)molecules and/or nanoobjects. Herein, we present a continuous protocell transformation from membrane‐less coacervates to membranized coacervates and, ultimately, to giant hybrid vesicles. This transformation process is orchestrated by altering the balance of non‐covalent interactions through varying concentrations of an anionic terpolymer, leading to dynamic processes such as spontaneous membranization of terpolymer nanoparticles at the coacervate surface, disassembly of the coacervate phase mediated by the excess anionic charge, and the redistribution of coacervate components in membrane. The diverse protocells during the transformation course provide distinct structural features and molecular permeability. Notably, the introduction of multiphase coacervates in this continuous transformation process signifies advancements toward the creation of synthetic cells with different diffusible compartments. Our findings emphasize the highly controlled continuous structural reorganization of coacervate protocells and represents a novel step toward the development of advanced and sophisticated synthetic protocells with more precise compositions and complex (membrane) structures.

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40

Kluczka, Eugénie, Valentin Rinaldo, Angélique Coutable-Pennarun, Claire Stines-Chaumeil, J. L. Ross Anderson, and Nicolas Martin. "Enhanced Catalytic Activity of a de novo Enzyme in a Coacervate Phase." ChemCatChem, May 8, 2024. http://dx.doi.org/10.1002/cctc.202400558.

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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 to study enzyme catalysis. Enzyme reactions within these droplets show altered kinetics, influenced by factors such as enzyme and substrate partitioning, crowding, and interactions with coacervate components; it is often challenging to disentangle the contributions of each. Here, we investigate the peroxidase activity of a de novo enzyme within polysaccharide‐based coacervates. By comparing the reaction kinetics in buffer, in a suspension of coacervates and in the bulk coacervate phase collected after centrifugation of the droplets, we show that the coacervate phase significantly increases the enzyme catalytic efficiency. We demonstrate that the main origin of this enhanced activity lies in macromolecular crowding coupled to changes in the conformational dynamics of the enzyme within the coacervate environment. Altogether, these findings underline the crucial role of the coacervate matrix in enzyme catalysis, beyond simple partitioning effects. The observed boost in enzyme activity within the coacervate phase provides insights for designing biocatalytically active synthetic organelles.

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41

Wang, Jiahua, Manzar Abbas, Yu Huang, Junyou Wang, and Yuehua Li. "Redox-responsive peptide-based complex coacervates as delivery vehicles with controlled release of proteinous drugs." Communications Chemistry 6, no. 1 (November 7, 2023). http://dx.doi.org/10.1038/s42004-023-01044-8.

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AbstractProteinous drugs are highly promising therapeutics to treat various diseases. However, they suffer from limited circulation times and severe off-target side effects. Inspired by active membraneless organelles capable of dynamic recruitment and releasing of specific proteins, here, we present the design of coacervates as therapeutic protocells, made from small metabolites (anionic molecules) and simple arginine-rich peptides (cationic motif) through liquid-liquid phase separation. These complex coacervates demonstrate that their assembly and disassembly can be regulated by redox chemistry, which helps to control the release of the therapeutic protein. A model proteinous drugs, tissue plasminogen activator (tPA), can rapidly compartmentalize inside the complex coacervates, and the coacervates formed from peptides conjugated with arginine-glycine-aspartic acid (RGD) motif (a fibrinogen-derived peptide sequence), show selective binding to the thrombus site and thus enhance on-target efficacy of tPA. Furthermore, the burst release of tPA can be controlled by the redox-induced dissolution of the coacervates. Our proof-of-principle complex coacervate system provides insights into the sequestration and release of proteinous drugs from advanced drug delivery systems and represents a step toward the construction of synthetic therapeutic protocells for biomedical applications.

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42

Chen, Hongfei, Yishu Bao, Xiaojing Li, Fangke Chen, Ryohichi Sugimura, Xiangze Zeng, and Jiang Xia. "Cell Surface Engineering by Phase‐Separated Coacervates for Antibody Display and Targeted Cancer Cell Therapy." Angewandte Chemie International Edition, August 5, 2024. http://dx.doi.org/10.1002/anie.202410566.

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Cell therapies such as CAR‐T have demonstrated significant clinical successes, driving the investigation of immune cell surface engineering using natural and synthetic materials to enhance their therapeutic performance. However, many of these materials do not fully replicate the dynamic nature of the extracellular matrix (ECM). This study presents a cell surface engineering strategy that utilizes phase‐separated peptide coacervates to decorate the surface of immune cells. We meticulously designed a tripeptide, Fmoc‐Lys‐Gly‐Dopa‐OH (KGdelta; Fmoc = fluorenylmethyloxycarbonyl; delta = Dopa, dihydroxyphenylalanine), that forms coacervates in aqueous solution via phase separation. These coacervates, mirroring the phase separation properties of ECM proteins, coat the natural killer (NK) cell surface with the assistance of Fe3+ ions and create an outer layer capable of encapsulating monoclonal antibodies (mAb), such as Trastuzumab. The antibody‐embedded coacervate layer equips the NK cells with the ability to recognize cancer cells and eliminate them through enhanced antibody‐dependent cellular cytotoxicity (ADCC). This work thus presents a unique strategy of cell surface functionalization and demonstrates its use in displaying cancer‐targeting mAb for cancer therapies, highlighting its potential application in the field of cancer therapy.

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43

Chen, Hongfei, Yishu Bao, Xiaojing Li, Fangke Chen, Ryohichi Sugimura, Xiangze Zeng, and Jiang Xia. "Cell Surface Engineering by Phase‐Separated Coacervates for Antibody Display and Targeted Cancer Cell Therapy." Angewandte Chemie, August 5, 2024. http://dx.doi.org/10.1002/ange.202410566.

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Cell therapies such as CAR‐T have demonstrated significant clinical successes, driving the investigation of immune cell surface engineering using natural and synthetic materials to enhance their therapeutic performance. However, many of these materials do not fully replicate the dynamic nature of the extracellular matrix (ECM). This study presents a cell surface engineering strategy that utilizes phase‐separated peptide coacervates to decorate the surface of immune cells. We meticulously designed a tripeptide, Fmoc‐Lys‐Gly‐Dopa‐OH (KGdelta; Fmoc = fluorenylmethyloxycarbonyl; delta = Dopa, dihydroxyphenylalanine), that forms coacervates in aqueous solution via phase separation. These coacervates, mirroring the phase separation properties of ECM proteins, coat the natural killer (NK) cell surface with the assistance of Fe3+ ions and create an outer layer capable of encapsulating monoclonal antibodies (mAb), such as Trastuzumab. The antibody‐embedded coacervate layer equips the NK cells with the ability to recognize cancer cells and eliminate them through enhanced antibody‐dependent cellular cytotoxicity (ADCC). This work thus presents a unique strategy of cell surface functionalization and demonstrates its use in displaying cancer‐targeting mAb for cancer therapies, highlighting its potential application in the field of cancer therapy.

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44

Blanco‐López, Marcos, Alejandro Marcos‐García, Álvaro González‐Garcinuño, Antonio Tabernero, and Eva M. Martín del Valle. "Exploring the effect of experimental conditions on the synthesis and stability of alginate–gelatin coacervates." Polymers for Advanced Technologies 35, no. 8 (August 2024). http://dx.doi.org/10.1002/pat.6554.

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AbstractAlginate–gelatin coacervation has been studied by considering different experimental parameters, such as gelatin preheating, pH, alginate–gelatin ratio and their respective concentrations, and salt effect. Results were assessed in terms of size and polydispersion via dynamic light scattering, electrostatic charge in the surface by zeta potential measurements, electrostatic interaction forces by static light scattering, stability by turbidimetry and viscoelastic and pseudoplastic behavior by rheology (oscillatory and statistical analysis). According to the results, gelatin structure has to be previously modified to induce the proper interactions with a subsequent pH reduction. Specifically, stable coacervates (according to turbidimetry and dynamic light scattering) with a size of 300–600 nm and a polydispersion lower than 0.25 were obtained after preheating the gelatin at 37°C and with a subsequent pH reduction until 4–5 for an alginate–gelatin ratio between 1:4 and 1:6. However, different experimental conditions promote an unsuccessful coacervation, obtaining always precipitates and/or coacervates with a wider particle size distribution. Furthermore, in order to study the effect of the temperature on the coacervates, different cooling–heating cycles were applied on them over a week, showing the stability of the thermo‐reversible coacervates for almost 5 days. Also, the interactions were characterized via static light scattering, analyzing the second virial coefficient. Moreover, rheological oscillatory results can be used to identify a proper coacervation due to the increase of the storage modulus. However, no significant changes were observed with statistical analysis due to the highly diluted character of the precursor solutions. These results highlighted how a proper combination of different experimental conditions, mainly temperature to promote a partial gelatin unraveling as well as pH reduction, is required to successfully produce coacervates. Finally, salt effect was proven to induce precipitation when NaCl was increasingly added to solutions of stable coacervates.

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45

Choi, Hyunsuk, Yuri Hong, Saeed Najafi, Sun Young Kim, Joan‐Emma Shea, Dong Soo Hwang, and Yoo Seong Choi. "Spontaneous Transition of Spherical Coacervate to Vesicle‐Like Compartment." Advanced Science, December 8, 2023. http://dx.doi.org/10.1002/advs.202305978.

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AbstractNumerous biological systems contain vesicle‐like biomolecular compartments without membranes, which contribute to diverse functions including gene regulation, stress response, signaling, and skin barrier formation. Coacervation, as a form of liquid–liquid phase separation (LLPS), is recognized as a representative precursor to the formation and assembly of membrane‐less vesicle‐like structures, although their formation mechanism remains unclear. In this study, a coacervation‐driven membrane‐less vesicle‐like structure is constructed using two proteins, GG1234 (an anionic intrinsically disordered protein) and bhBMP‐2 (a bioengineered human bone morphogenetic protein 2). GG1234 formed both simple coacervates by itself and complex coacervates with the relatively cationic bhBMP‐2 under acidic conditions. Upon addition of dissolved bhBMP‐2 to the simple coacervates of GG1234, a phase transition from spherical simple coacervates to vesicular condensates occurred via the interactions between GG1234 and bhBMP‐2 on the surface of the highly viscoelastic GG1234 simple coacervates. Furthermore, the shell structure in the outer region of the GG1234/bhBMP‐2 vesicular condensates exhibited gel‐like properties, leading to the formation of multiphasic vesicle‐like compartments. A potential mechanism is proposed for the formation of the membrane‐less GG1234/bhBMP‐2 vesicle‐like compartments. This study provides a dynamic process underlying the formation of biomolecular multiphasic condensates, thereby enhancing the understanding of these biomolecular structures.

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46

Nair, Karthika S., Sreelakshmi Radhakrishnan, and Harsha Bajaj. "Dynamic Control of Functional Coacervates in Synthetic Cells." ACS Synthetic Biology, June 19, 2023. http://dx.doi.org/10.1021/acssynbio.3c00249.

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47

Späth, Fabian, Anton S. Maier, Michele Stasi, Alexander M. Bergmann, Kerstin Halama, Monika Wenisch, Bernhard Rieger, and Job Boekhoven. "The Role of Chemically Innocent Polyanions in Active, Chemically Fueled Complex Coacervates." Angewandte Chemie International Edition, August 7, 2023. http://dx.doi.org/10.1002/anie.202309318.

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Complex coacervation describes the liquid‐liquid phase separation of oppositely charged polymers. Active coacervates are droplets in which one of the electrolyte´s affinity is regulated by chemical reactions. These droplets are particularly interesting because they are tightly regulated by reaction kinetics. For example, they serve as a model for membraneless organelles that are also often regulated by biochemical transformations such as posttranslational modifications. They are also a great protocell model or could be used to synthesize life—they spontaneously emerge in response to reagents, compete, and decay when all nutrients have been consumed. However, the role of the unreactive building blocks, e.g., the polymeric compounds, is poorly understood. Here, we show the important role of the chemically innocent, unreactive polyanion of our chemically fueled coacervation droplets. We show that the polyanion drastically influences the resulting droplets' life cycle without influencing the chemical reaction cycle—either they are very dynamic or have a delayed dissolution. Additionally, we derive a mechanistic understanding of our observations and show how additives and rational polymer design help to create the desired coacervate emulsion life cycles.

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48

Späth, Fabian, Anton S. Maier, Michele Stasi, Alexander M. Bergmann, Kerstin Halama, Monika Wenisch, Bernhard Rieger, and Job Boekhoven. "The Role of Chemically Innocent Polyanions in Active, Chemically Fueled Complex Coacervates." Angewandte Chemie, August 7, 2023. http://dx.doi.org/10.1002/ange.202309318.

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Complex coacervation describes the liquid‐liquid phase separation of oppositely charged polymers. Active coacervates are droplets in which one of the electrolyte´s affinity is regulated by chemical reactions. These droplets are particularly interesting because they are tightly regulated by reaction kinetics. For example, they serve as a model for membraneless organelles that are also often regulated by biochemical transformations such as posttranslational modifications. They are also a great protocell model or could be used to synthesize life—they spontaneously emerge in response to reagents, compete, and decay when all nutrients have been consumed. However, the role of the unreactive building blocks, e.g., the polymeric compounds, is poorly understood. Here, we show the important role of the chemically innocent, unreactive polyanion of our chemically fueled coacervation droplets. We show that the polyanion drastically influences the resulting droplets' life cycle without influencing the chemical reaction cycle—either they are very dynamic or have a delayed dissolution. Additionally, we derive a mechanistic understanding of our observations and show how additives and rational polymer design help to create the desired coacervate emulsion life cycles.

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49

Kishimura, Akihiro, Biplab K C, Teruki Nii, Takeshi Mori, and Yoshiki Katayama. "Dynamic frustrated charge hotspots created by charge density modulation sequester globular proteins into complex coacervates." Chemical Science, 2023. http://dx.doi.org/10.1039/d3sc00993a.

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This study presents a simple strategy for the sequestration of globular proteins as clients into synthetic polypeptide-based complex coacervates as a scaffold, thereby recapitulating the scaffold-client interaction found in biological...

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50

Ardestani, Faezeh, Ali Haghighi Asl, and Ali Rafe. "Characterization of caseinate-pectin complex coacervates as a carrier for delivery and controlled-release of saffron extract." Chemical and Biological Technologies in Agriculture 11, no. 1 (August 21, 2024). http://dx.doi.org/10.1186/s40538-024-00647-0.

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AbstractIn this work, microcapsules were developed by the complex coacervation of sodium caseinate and pectin as a carrier for saffron extract. Parameters such as Zeta potential, dynamic light scattering, and microscopic techniques were investigated for their influence on the formation of these complexes. Furthermore, Fourier transform infrared (FTIR) analysis confirmed the reaction mechanism between the protein and tannic acid or saffron extract. The study revealed that core/shell and protein/polysaccharide (Pr/Ps) ratios play a role in the encapsulation efficiency (EE) and loading capacity (LC) of saffron extract, with EE and LC ranging from 48.36 to 89.38% and 1.14 to 5.55%, respectively. Thermal gravimetric analysis revealed that the degradation temperature of saffron increased significantly with microencapsulation. The use of tannic acid for hardening the microcapsules led to an increase in size from 13 μm to 27 μm. Rheological findings indicated that shear-thinning behavior in the coacervates, with cross-linking, has a minor effect on the interconnected elastic gel structures. However, cross-linking improved the microcapsules' thermal and structural properties. The increase in polymer chain length due to cross-linking and the presence of the guest molecule (saffron extract) resulted in higher rheological moduli, reflecting enhanced entanglements and correlating well with the thermal, structural, and microstructural properties of the coacervates. Kinetic release studies showed a slower release in the gastric phase compared to the intestinal phase, with the Ritger–Peppas model effectively describing saffron extract release, highlighting a dominant swelling and dissolution release mechanism. Therefore, the NaCas/HMP coacervate wall materials made saffron stable in the gastric stage and sustainably release. It in the intestinal stage, promoting excellent absorption of saffron in simulated digestion. Graphical Abstract

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