Bioinspired Autocatalysis for Polymer Nanoparticle Synthesis: Monomer Preassembly through Liquid–Liquid Phase Separation DOI
Ying Cao, Ran Zhang, Xiaoyue Xu

et al.

Macromolecules, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 15, 2024

Biomimetic synthesis represents a cutting-edge topic in chemical and materials sciences. Herein, we present an approach to bioinspired polymerization autocatalysis using single amino acid monomer water. Similar biomolecular condensates, this undergoes entropically driven liquid–liquid phase separation (LLPS)-mode self-assembly involving densely charged molecular clusters formation, LLPS of leading submicron-scale droplets, crystallization within droplet crowding environments resulting dynamic nanocrystals@droplets finally less aged-lamellae. Supramolecular chirality inversion nanocrystal disassembly into occur upon doping minor RAFT agent. Autocatalysis with solvent-tuned H+-feedback covalent-driven is achieved extremely nanocrystals@droplets. Decelerated kinetics deionization/ion-pairing underscore the vital importance for "higher charge repulsion leads more rapid polymerization", yielding polymer nanoparticles protein-like structural complexity up >98% conversion 2-min-propagation period. This provides new insights efficient nanoparticles.

Language: Английский

Chiral Induced Spin Selectivity DOI Creative Commons
Brian P. Bloom, Yossi Paltiel, Ron Naaman

et al.

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(4), P. 1950 - 1991

Published: Feb. 16, 2024

Since the initial landmark study on chiral induced spin selectivity (CISS) effect in 1999, considerable experimental and theoretical efforts have been made to understand physical underpinnings mechanistic features of this interesting phenomenon. As first formulated, CISS refers innate ability materials act as filters for electron transport; however, more recent experiments demonstrate that displacement currents arising from charge polarization molecules lead without need net flow. With its identification a fundamental connection between symmetry materials, promises profound ubiquitous implications existing technologies new approaches answering age old questions, such homochiral nature life. This review begins with discussion different methods measuring then provides comprehensive overview known exhibit CISS-based phenomena before proceeding identify structure-property relations delineate leading models effect. Next, it identifies some physics, chemistry, biology. The ends critical assessment field comments future outlook.

Language: Английский

Citations

122
A Chemical Reaction Network Drives Complex Population Dynamics in Oscillating Self-Reproducing Vesicles DOI
Zhiheng Zhang, Michael G. Howlett, Emma Silvester

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(27), P. 18262 - 18269

Published: June 25, 2024

We report chemically fueled oscillations of vesicles. The population cycling vesicles is driven by their self-reproduction and collapse within a biphasic reaction network involving the interplay molecular supramolecular events. studied on scales tracked vesicle populations in time interferometric scattering microscopy dynamic light scattering. Complex events were observed during oscillations─including reproduction, growth, decomposition─and differences number, size, mass aggregates can often be between pulses. This system's behavior reminiscent reproductive cycle living cells.

Language: Английский

Citations

7
Cysteine‐Based Dynamic Self‐Assembly and Their Importance in the Origins of Life DOI
Soumen Kuila, Jayanta Nanda

ChemSystemsChem, Journal Year: 2024, Volume and Issue: 6(4)

Published: April 12, 2024

Abstract The knowledge regarding the origins of life from inanimate materials is still elusive. It was proposed that biological building blocks evolved inorganic substances present in early earth conditions. However, process by which chemistry can be converted into biology has not yet been achieved laboratory. artificial system out‐of‐equilibrium state must maintain a few critical features life, like compartmentalization, metabolism, and replication, to considered alive. In this direction, working with cysteine (Cys)‐based molecules strategic understand evolution process. presence sulphydryl (−SH) group Cys‐residue build dynamic equilibrium through disulfide redox under proper guidance oxidizing reducing agents. review article, our primary focus discuss Cys‐containing short‐peptide‐based self‐assembly disassembly processes. formation bonds sometimes helps gelation, but reverse also true some cases. later part we cover fact these sulphydryl‐based systems have shown their adaptability mimic different life‐essential criteria participate Darwinian evolution.

Language: Английский

Citations

5
Crosstalk between DNA Damage Repair and Metabolic Regulation in Hematopoietic Stem Cells DOI Creative Commons
Jian Xu,

Peiwen Fei,

Dennis Simon

et al.

Cells, Journal Year: 2024, Volume and Issue: 13(9), P. 733 - 733

Published: April 24, 2024

Self-renewal and differentiation are two characteristics of hematopoietic stem cells (HSCs). Under steady physiological conditions, most primitive HSCs remain quiescent in the bone marrow (BM). They respond to different stimuli refresh blood system. The transition from quiescence activation is accompanied by major changes metabolism, a fundamental cellular process living organisms that produces or consumes energy. Cellular metabolism now considered be key regulator HSC maintenance. Interestingly, possess distinct metabolic profile with preference for glycolysis rather than oxidative phosphorylation (OXPHOS) energy production. Byproducts can also damage DNA. To counteract such insults, mammalian have evolved complex efficient DNA repair (DDR) system eliminate various lesions guard genomic stability. Given enormous regenerative potential coupled lifetime persistence HSCs, tight control genome stability essential. intersection DDR has recently emerged as an area intense research interest, unraveling profound connections between energetics. In this brief review, we delve into interplay deficiency reprogramming shedding light on dynamic relationship governs fate functionality these remarkable cells. Understanding crosstalk will open new avenue designed target interacting pathways improving function treating hematologic disorders.

Language: Английский

Citations

4
CO2-fueled non-equilibrium supramolecular gels as gas-encoded information encryption materials DOI
Yulian Zhang, Xin Liang, Qiang Yan

et al.

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: March 12, 2025

Language: Английский

Citations

0
Designing supramolecular catalytic systems for mammalian synthetic metabolism DOI
Jingjing Han, Martin Fussenegger

Nature Reviews Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 29, 2025

Language: Английский

Citations

0
The GARD Prebiotic Reproduction Model Described in Order and Complexity DOI Creative Commons
Christian Mayer, Doron Lancet, Omer Markovitch

et al.

Life, Journal Year: 2024, Volume and Issue: 14(3), P. 288 - 288

Published: Feb. 21, 2024

Early steps in the origin of life were necessarily connected to unlikely formation self-reproducing structures from chaotic chemistry. Simulations chemical kinetics based on graded autocatalysis replication domain (GARD) model demonstrate ability a micellar system become units away equilibrium. Even though they may be very rare initial state system, property their endogenous mutually catalytic networks being dynamic attractors greatly enhanced reproduction propensity, revealing potential for selection and Darwinian evolution processes. In parallel, order complexity have been shown crucial parameters successful evolution. Here, we probe these dynamics GARD-governed entities an attempt identify characteristic mechanisms development non-covalent molecular assemblies. Using virtual random walk perspective, value consecutive is defined statistical thermodynamics. The complexity, other hand, determined by size minimal algorithm fully describing properties walk. By referring previously published diagonal line order/complexity diagram that represents progression evolution, it GARD has advance this direction. These results can serve as solid foundation identifying general criteria future analyses evolving systems.

Language: Английский

Citations

3
The astrochemical evolutionary traits of phospholipid membrane homochirality DOI
Jana Bocková, Nykola C. Jones, Søren Vrønning Hoffmann

et al.

Nature Reviews Chemistry, Journal Year: 2024, Volume and Issue: 8(9), P. 652 - 664

Published: July 18, 2024

Language: Английский

Citations

3
Nonequilibrium Membrane Dynamics Induced by Active Protein Interactions and Chemical Reactions: A Review DOI Creative Commons
Hiroshi Noguchi

ChemSystemsChem, Journal Year: 2024, Volume and Issue: unknown

Published: July 22, 2024

Abstract Biomembranes wrapping cells and organelles are not only the partitions that separate insides but also dynamic fields for biological functions accompanied by membrane shape changes. In this review, we discuss spatiotemporal patterns fluctuations of membranes under nonequilibrium conditions. particular, focus on theoretical analyses simulations. Protein active forces enhance or suppress fluctuations; height spectra deviated from thermal spectra. binding unbinding to is activated inhibited other proteins chemical reactions, such as ATP hydrolysis. Such processes can induce traveling waves, Turing patterns, morphological They be represented continuum reaction‐diffusion equations discrete lattice/particle models with state flips. The effects structural changes in amphiphilic molecules molecular‐assembly structures discussed.

Language: Английский

Citations

3
Site-Specific Polymerization-Induced Electrostatic Self-Assembly: Synthesis of Highly Charged Salt-Tolerant Polyion Complex Nanoreactors DOI
Jie Cai, Xiyu Wang, Yuanyuan Liu

et al.

Macromolecules, Journal Year: 2023, Volume and Issue: 56(24), P. 10153 - 10162

Published: Dec. 5, 2023

We herein report a site-specific polymerization-induced electrostatic self-assembly (PIESA) that enables the precision synthesis of highly charged salt-tolerant nanoreactors. Site-specific PIESA is achieved using an anionic aromatic–aliphatic sulfonate block copolymer in photoinitiated reversible addition-fragmentation chain transfter (photo-RAFT) polymerization cationic monomer water at 25 °C. Preferential complexation growing chains to aromatic results not only molecular recognition but also unique PIC nanoparticles. Neutral incorporation leads ultrafast reaction very dilute (2.0% w/w) and exclusive formation more smaller spheres or 4 nm fibril-structured 10 ultrathin lamellae. The lamellae can induce sequence-controllable copolymerization oppositely-charged monomers with perfect shape/size preservation up 100% conversions, thus be viewed as nanoreactor. This work opened avenue for functional nanoparticles, providing versatile platform easy access structural complexity from simple mixtures.

Language: Английский

Citations

6