The chemistry of chemically fueled droplets

Donau, Carsten; Boekhoven, Job

doi:10.1016/j.trechm.2022.11.003

Cited by 30 publications

(15 citation statements)

References 87 publications

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“…Taking a reported diffusion coefficient of 81 for an amphiphilic diblock copolymer with R e ∼10 2 nm yields a common self-diffusion time of τ 0 ∼ 10 −2 s and hence the presented simulations cover times of t ∼ 30 s. The corresponding deactivation times in our case would be on the order of for the slowest reaction rates. Commonly reported values of 82 are higher, implying the lattice spacing would increase by a factor of . Notice, that lower molecular weights will require higher reaction rates.…”

Section: Discussionmentioning

confidence: 98%

Reaction-driven assembly: controlling changes in membrane topology by reaction cycles

Häfner,

Müller

2023

Soft Matter

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Section: Discussionmentioning

confidence: 98%

Reaction-driven assembly: controlling changes in membrane topology by reaction cycles

Häfner,

Müller

2023

Soft Matter

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“…Their high-water content makes them especially appealing for the microencapsulation of hydrophilic substances, e.g., proteins, polynucleotides, or ionic drugs. It also makes them a great model for membraneless organelles or protocells . Compared to complex coacervates comprising a mixture of oppositely charged polyelectrolytes, hydrophobic interactions of amphiphilic molecules or polymers can initiate micelle formation.…”

Section: The Design Of Chemically Fueled Supramolecular Materialsmentioning

confidence: 99%

Chemically Fueled Supramolecular Materials

2023

Self Cite

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Metrics & MoreArticle Recommendations CONSPECTUS:In biology, the function of many molecules is regulated through nonequilibrium chemical reaction cycles. The prototypical example is the phosphorylation of an amino acid in an enzyme which induces a functional change, e.g., it folds or unfolds, assembles or disassembles, or binds a substrate. Such phosphorylation does not occur spontaneously but requires a phosphorylating agent with high chemical potential (for example, adenosine triphosphate (ATP)) to be converted into a molecule with lower chemical potential (adenosine diphosphate (ADP)). When this energy is used to regulate an assembly, we speak of chemically fueled assemblies; i.e., the molecule with high potential, the fuel, is used to regulate a self-assembly process. For example, the binding of guanosine triphosphate (GTP) to tubulin induces self-assembly. The bound GTP is hydrolyzed to guanosine diphosphate (GDP) upon assembly, which induces tubulin disassembly.The result is a dynamic assembly endowed with unique characteristics, such as time-dependent behavior and the ability to self-heal. These intriguing, unique properties have inspired supramolecular chemists to create similar chemically fueled molecular assemblies from the bottom up. While examples have been designed, they remain scarce partly because chemically fueled reaction cycles are rare and often complex. Thus, we recently developed a carbodiimide-driven reaction cycle that is versatile and easy to use, quantitatively understood, and does not suffer from side reactions. In the reaction cycle, a carboxylate precursor reacts with a carbodiimide to form an activated species like an anhydride or ester. The activated state reacts with water and thereby reverts to its precursor state; i.e., the activated state is deactivated. Effectively, the precursor catalyzes carbodiimides' conversion into waste and forms a transient activated state.We designed building blocks to regulate a range of assemblies and supramolecular materials at the expense of carbodiimide fuel. The simplicity and versatility of the reaction cycles have democratized and popularized the field of chemically fueled assemblies. In this Account, we describe what we have "learned" on our way. We introduce the field exemplified by biological nonequilibrium selfassembly. We describe the design of the carbodiimide-driven reaction cycle. Using examples from our group and others, we offer design rules for the building block's structure and strategies to create the desired morphology or supramolecular materials. The discussed morphologies include fibers, colloids, crystals, and oil-and coacervate-based droplets. We then demonstrate how these assemblies form supramolecular materials with unique material properties like the ability to self-heal. Besides, we discuss the concept of reciprocal coupling in which the assembly exerts feedback on its reaction cycle and we also offer examples of such feedback mechanisms. Finally, we close the Account with a discussion and an outlook on this field. This Acco...

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“…Similarly, recent work shows chemical fuels regulating different aspects of primitive coacervation. [ 163 ] Is there a way that active droplets could divide through similar modulation of surface tension [ 25 ] or charge?…”

Section: Aspects Of Primitive Llpsmentioning

confidence: 99%

A compositional view comparing modern biological condensates and primitive phase‐separated compartments

Cannelli,

Gupta,

Nguyen

et al. 2023

Peptide Science

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Liquid–liquid phase separation (LLPS) is a process that often occurs due to binding between oppositely charged biopolymers, and has gained increasing attention recently due to their ubiquity in biological systems and ability to direct essential cellular processes. However, while these discoveries in biology are recent, the field of origins of life has been investigating LLPS for nearly 100 years, ever since the first suggestions by Oparin and Haldane that primitive LLPS could have been precursors to the first cells on Earth. Since then, a significant amount of work has been done to elucidate different primitive LLPS systems that could have been relevant as protocellular models. Given the structural similarities between primitive LLPS and modern membraneless organelles, there may even be an evolutionary link between the two, although this remains a question to be answered. Nevertheless, in order to answer this, a source that compares compositional aspects of modern biological condensates and primitive LLPS is necessary. Here, we first focus on membraneless organelles composed of intrinsically disordered proteins (IDPs) and nucleic acids. Then, as a parallel, we explore primitive membraneless compartments composed of simple biopolymers such as short peptides and nucleic acids. This is followed by a discussion of how the first biomolecules on Earth may have originated, analyzing the environmental and chemical conditions that could have favored primitive LLPS processes. Finally, we directly compare composition of modern biological condensates and primitive phase‐separated compartments, further discussing the potential of primitive IDPs on early Earth, but also the evolution from membraneless to membrane‐bound cells. This review aims to provide a compositional comparison of modern and primitive phase‐separated structures in order to help researchers in both fields understand the current state of knowledge, how this knowledge evolved, and the current gaps that need to be further addressed.

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The chemistry of chemically fueled droplets

Cited by 30 publications

References 87 publications

Reaction-driven assembly: controlling changes in membrane topology by reaction cycles

Reaction-driven assembly: controlling changes in membrane topology by reaction cycles

Chemically Fueled Supramolecular Materials

A compositional view comparing modern biological condensates and primitive phase‐separated compartments

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