Parasitic behavior in competing chemically fueled reaction cycles

Schwarz, Patrick; Laha, Sudarshana; Janssen, Jacqueline; Huss, Tabea; Boekhoven, Job; Weber, Christoph A.

doi:10.1039/d1sc01106e

Cited by 17 publications

(14 citation statements)

References 57 publications

(65 reference statements)

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“…These models differ from the binary model by taking into account a solvent S which phase-separates from the droplet material D. Most importantly, this solvent does not undergo chemical transitions with the droplet material D. Therefore, the proposed models in our work are closer to existing experimental systems. [16][17][18][19] As we will show in the following, our simple protocell models also exhibit regimes where droplets are stable with a finite size, and regimes where droplets divide via a shape instability. Examples of droplet dynamics in the boundary driven case are shown in Figure 2 as snapshots of configurations of droplet material at N .…”

Section: Droplet Dynamics and Droplet Divisionmentioning

confidence: 72%

“…Such experimental systems typically involve multiple components that undergo chemical reactions. [ 16–19 ] As our work shows, simply providing energy via a fuel is not sufficient to drive growth, because growth requires the accumulation of a conserved quantity. Similarly, cycles of droplet growth and division also requires the supply of a conserved quantity.…”

Section: Discussionmentioning

confidence: 96%

“…These scenarios distinguish between nutrient, droplet material, waste, and solvent. Such systems are versatile and open new possibilities for experimental realizations since real chemical systems with active droplets [16][17][18][19] are not binary and the spatial distribution of nutrients and waste is in general relevant for the emergence of the aforementioned life-like behaviors. Droplet systems also provide appealing models of simple but realistic protocells and permit to consider both energy and matter flows.…”

Section: Introductionmentioning

confidence: 99%

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Energy and Matter Supply for Active Droplets

2022

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Chemically active droplets provide simple models for cell‐like systems that can grow and divide. Such active droplet systems are driven away from thermodynamic equilibrium and turn over chemically, which corresponds to a simple metabolism. Two scenarios of nonequilibrium driving are considered. First, droplets are driven via the system boundaries by external reservoirs that supply nutrient and remove waste (boundary‐driven). Second, droplets are driven by a chemical energy provided by a fuel in the bulk (bulk‐driven). For both scenarios, the conservation of energy and matter as well as the balance of entropy are discussed. Conserved and nonconserved fields are used to analyse the nonequilibrium steady states of active droplets. Using an effective droplet model, droplet stability and instabilities leading to droplet division are explored. This work reveals that droplet division occurs quite generally in active droplet systems. The results suggest that life‐like processes such as metabolism and division can emerge in simple nonequilibrium systems that combine the physics of phase separation and chemical reactions.

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Section: Droplet Dynamics and Droplet Divisionmentioning

confidence: 72%

Section: Discussionmentioning

confidence: 96%

Section: Introductionmentioning

confidence: 99%

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Energy and Matter Supply for Active Droplets

2022

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“…High-performance liquid chromatography (HPLC) studies allowed us to capture the evolution of the all-reactive species in the reaction cycle . The rate constants of the involved chemical reactions could be calculated and used in a kinetic model that accurately predicts the evolution of the concentrations of the relevant chemical species and their reaction rates.…”

Section: Introductionmentioning

confidence: 99%

“…High-performance liquid chromatography (HPLC) studies allowed us to capture the evolution of the all-reactive species in the reaction cycle. 36 The rate constants of the involved chemical reactions could be calculated and used in a kinetic model that accurately predicts the evolution of the The mechanisms governing the time-dependent behavior of the size distribution of chemically regulated droplets were addressed recently using various 2-alkenyl-succinates. 37 The evolution of the droplet size and its distribution was determined by confocal microscopy.…”

Section: Introductionmentioning

confidence: 99%

Droplet Formation by Chemically Fueled Self-Assembly: The Role of Precursor Hydrophobicity

et al. 2021

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We investigate active droplets that form at the expense of a chemical fuel in aqueous buffer and vanish autonomously. Dynamic light scattering reveals the scattered intensity, the hydrodynamic radius, and the width of the size distribution with high precision as well as high temporal and spatial resolutions. Comparing the resulting time-dependent behavior of the droplet characteristics with the time-dependent concentration of the anhydrides, the roles of the chemical reaction cycle and of colloidal growth processes are elucidated. The droplet sizes and lifetimes depend strongly on the hydrophobicity of the precursor, and the growth rate is found to correlate with the deactivation rate of the product.

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Out‐of‐equilibrium supramolecular self‐assembling systems driven by chemical fuel

Wang

Chen

et al. 2021

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A rich variety of smart materials developed via supramolecular assembly strategies have been introduced in the past decades. However, most materials reside in the thermodynamic equilibrium state, opposed to those nonequilibrium structures with sophisticated functions that are observed in living systems. To develop advanced synthetic systems, chemists have begun to focus on how to use strategies similar to those used in biological systems for fabricating artificial out-of-equilibrium systems. Heretofore, a rich variety of artificial out-of-equilibrium systems have been developed. In this review, we have summarized the recent progress of artificial out-of-equilibrium systems and categorized them in terms of the chemical fuel used, including adenosine triphosphate (ATP), acid/base, carbodiimide reagents, and many others. For these self-assembling systems, their design strategies, potential applications, as well as advantageous features have been discussed. At the end of this review, the remaining challenges and an outlook of the chemical-fuel-driven out-of-equilibrium systems were also discussed. It is believed that this review has provided some insights and could be useful for those who are interested in the out-of-equilibrium supramolecular assembling systems and their subsequent constructing strategies for various transient materials.

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Parasitic behavior in competing chemically fueled reaction cycles

Abstract: Non-equilibrium, fuel-driven reaction cycles serve as model systems of the intricate reaction networks of life. Rich and dynamic behavior is observed when reaction cycles regulate assembly processes, such as phase...

Cited by 17 publications

References 57 publications

Energy and Matter Supply for Active Droplets

Energy and Matter Supply for Active Droplets

Droplet Formation by Chemically Fueled Self-Assembly: The Role of Precursor Hydrophobicity

Out‐of‐equilibrium supramolecular self‐assembling systems driven by chemical fuel

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