Bioreactor droplets from liposome-stabilized all-aqueous emulsions

Dewey, Daniel C.; Strulson, Christopher A.; Cacace, David N.; Bevilacqua, Philip C.; Keating, Christine D.

doi:10.1038/ncomms5670

Cited by 234 publications

(245 citation statements)

References 52 publications

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“…Compartments efficiently restrict the diffusion of reactive species 35 , but conversely require specific strategies in order to open communication channels between the units [36][37][38][39] . Living organisms elegantly manage transfer across their boundaries.…”

Section: Resultsmentioning

confidence: 99%

Microscopic agents programmed by DNA circuits

Gines¹,

Zadorin²,

Galas³

et al. 2017

Nature Nanotech

125

148

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Section: Resultsmentioning

confidence: 99%

Microscopic agents programmed by DNA circuits

Gines¹,

Zadorin²,

Galas³

et al. 2017

Nature Nanotech

125

148

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“…These structures are formed when ~100 nm diameter lipid vesicles (large unilamellar vesicles, or LUVs) self-assemble at 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 -4 -the aqueous/aqueous interface of a PEG/dextran biphasic system [29][30][31][32] , stabilizing enzyme-loaded droplets of dextran-rich phase in a continuous medium of PEG-rich phase. 33 and does not require membrane transporters or pore-forming molecules. 33 The combination of lipidstabilized, enzyme-loaded all-aqueous emulsion droplets with intermediate chelation provides excellent control over the mineralization process, enabling high-yield production of relatively monodisperse AMV populations.…”

Section: -27mentioning

confidence: 98%

“…33 and does not require membrane transporters or pore-forming molecules. 33 The combination of lipidstabilized, enzyme-loaded all-aqueous emulsion droplets with intermediate chelation provides excellent control over the mineralization process, enabling high-yield production of relatively monodisperse AMV populations. 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 Scheme 1.…”

Section: -27mentioning

confidence: 98%

Aqueous Emulsion Droplets Stabilized by Lipid Vesicles as Microcompartments for Biomimetic Mineralization

et al. 2015

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Mineral deposition within living cells relies on control over the distribution and availability of precursors as well as the location and rates of nucleation and growth. This control is provided in large part by biomolecular chelators, which bind precursors and regulate their availability, and compartmentalization within specialized mineralizing vesicles. Biomimetic mineralization in self-assembled lipid vesicles is an attractive means of studying the mineralization process, but has proven challenging due to vesicle heterogeneity in lamellarity, contents, and size across a population, difficulties encapsulating high and uniform precursor concentrations, and the need to transport reagents across an intact lipid bilayer membrane. Here, we report the use of liposome-stabilized all-aqueous emulsion droplets as simple artificial mineralizing vesicles (AMVs). These biomimetic microreactors allow the entry of precursors while retaining a protein catalyst by equilibrium partitioning between internal and external polymer-rich phases. Small molecule chelators with intermediate binding affinity were employed to control Ca(2+) availability during CaCO3 mineralization, providing protection against liposome aggregation while allowing CaCO3 formation. Mineral deposition was limited to the AMV interior, due to localized production of CO3(2-) by compartmentalized urease. Particle formation was uniform across the entire population of AMVs, with multiple submicrometer amorphous CaCO3 particles produced in each one. The all-aqueous emulsion-based approach to biomimetic giant mineral deposition vesicles introduced here should be adaptable for enzyme-catalyzed synthesis of a wide variety of materials, by varying the metal ion, enzyme, and/or chelator.

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“…Candidates for early-Earth compartments include crevices or pores in rocks 17 , self-assemblies of lipids or simpler amphiphiles to form vesicles 18–23 , and aqueous droplets formed by liquid-liquid phase separation 15, 21, 24 . Combining catalytic mineral surfaces with compartments such as amphiphile vesicles or droplets formed by aqueous/aqueous phase coexistence is therefore appealing as primitive protocell models.…”

Section: Introductionmentioning

confidence: 99%

“…The immiscible aqueous phases that result upon demixing in aqueous polymer solutions provide compartments with different chemical and physical properties between which solutes such as biomolecules (or their prebiotic precursors) can partition. Consequently, aqueous two-phase systems (ATPS) have been used for biomolecule separations 25, 26 , food science 27, 28 , and biomimetic compartmentalization 16, 18, 29 , and have been proposed as simple protocell models 15, 24, 30 .…”

Section: Introductionmentioning

confidence: 99%

Combining Catalytic Microparticles with Droplets Formed by Phase Coexistence: Adsorption and Activity of Natural Clays at the Aqueous/Aqueous Interface

Cakmak

Keating

2017

Sci Rep

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Natural clay particles have been hypothesized as catalysts on the early Earth, potentially facilitating the formation of early organic (bio) molecules. Association of clay particles with droplets formed by liquidliquid phase separation could provide a physical mechanism for compartmentalization of inorganic catalysts in primitive protocells. Here we explore the distribution of natural clay mineral particles in poly(ethylene glycol) (PEG)/dextran (Dx) aqueous two-phase systems (ATPS). We compared the three main types of natural clay: kaolinite, montmorillonite and illite, all of which are aluminosilicates of similar composition and surface charge. The three clay types differ in particle size, crystal structure, and their accumulation at the ATPS interface and ability to stabilize droplets against coalescence. Illite and kaolinite accumulated at the aqueous/aqueous interface, stabilizing droplets against coalescence but not preventing their eventual sedimentation due to the mass of adsorbed particles. The ability of each clay-containing ATPS to catalyze reaction of o-phenylenediamine with peroxide to form 2,3-diaminophenazone was evaluated. We observed modest rate increases for this reaction in the presence of clay-containing ATPS over clay in buffer alone, with illite outperforming the other clays. These findings are encouraging because they support the potential of combining catalytic mineral particles with aqueous microcompartments to form primitive microreactors.Clay minerals, which are composed of aluminosilicates with layered structures, are major components of soils and sedimentary rocks and among the most abundant minerals at the surface of the Earth 1 . Clays have found a wide variety of applications since ancient times including ceramics 2 , electrochemistry 3 , organoclay/polymer nanocomposites 4 and as catalysts in chemical reactions [5][6][7] . The availability of clay minerals and their potential for catalytic activity led to the proposal of these materials as inorganic catalysts for chemical evolution of biomolecules on the early Earth 8 . Since then clay particles have been demonstrated as catalysts for polymerization of activated nucleotides and amino acids 9 , lipid self-organization 10-12 and many other possible prebiotic reactions 11,13,14 .An important step in the transition from nonliving towards living matter is thought to be compartmentalization of molecules and of reactions 15,16 . Candidates for early-Earth compartments include crevices or pores in rocks 17 , self-assemblies of lipids or simpler amphiphiles to form vesicles [18][19][20][21][22][23] , and aqueous droplets formed by liquid-liquid phase separation 15,21,24 . Combining catalytic mineral surfaces with compartments such as amphiphile vesicles or droplets formed by aqueous/aqueous phase coexistence is therefore appealing as primitive protocell models. Szostak and coworkers reported that clay minerals accelerate the spontaneous conversion of fatty acid micelles into vesicles and some clay might get encapsulated within the vesicle...

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Bioreactor droplets from liposome-stabilized all-aqueous emulsions

Cited by 234 publications

References 52 publications

Microscopic agents programmed by DNA circuits

Microscopic agents programmed by DNA circuits

Aqueous Emulsion Droplets Stabilized by Lipid Vesicles as Microcompartments for Biomimetic Mineralization

Combining Catalytic Microparticles with Droplets Formed by Phase Coexistence: Adsorption and Activity of Natural Clays at the Aqueous/Aqueous Interface

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