Fuel‐driven π‐conjugated Superstructures to Form Transient Conductive Hydrogels DOI
Ifigeneia Tsironi, Jarek A. Maleszka,

Brigitte A. K. Kriebish

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 21, 2024

Abstract Despite advances in creating dissipative materials with transient properties, such as hydrogels and active droplets, their application remains confined to temporal changes structural properties. Developing out‐of‐equilibrium whose electronic functions are parameterized by a chemical reaction cycle is challenging. Yet, this class of required construct biomimetic materials. In contrast traditional cycles that exploit molecularly dissolved building blocks at thermodynamic equilibrium, we show fiber structures derived from reactive naphthalene diimide (NDI) can be used resting states form far‐from‐equilibrium conductive after the addition fuels. Upon fueling NDI‐derived fibers, dual‐component activation deactivation pathway deduced kinetic analysis absent when using state. Investigating solid‐state morphologies formed throughout fuel‐driven cryo‐EM reveals fibers evolve thicker fibrils layered superstructures. We redox‐active exhibit nearly threefold increase electrical conductivity upon fuel consumption before reverting original value over hours. These potential candidates applications programmable biorobotics computing.

Language: Английский

Pathway-Dependent Catalytic Activity of Short-Peptide-Based Metallozyme: From Promiscuous Activity to Cascade Reaction DOI

Chiranjit Mahato,

Sumit Pal, Himangshu Kuiry

et al.

Nano Letters, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 2, 2025

Many natural enzymes contain metal ions as cofactors in the active site for biological activity. However, pathway of introduction earliest protein folds emergence higher catalytic activity remains an intriguing open question. Herein, we demonstrate that pathway-dependent self-assembly short-peptide-based metallozymes results differences Short-peptide-based amyloids with solvent exposed arrays colocalized units are able to bind highly soluble Cu2+ oxidase-like and RNase-like (promiscuity). Further, metallozyme was exhibit hydrolase-oxidase cascade compared mixture enzymes, esterase, laccase. The collaboration between amyloid microphases suggests might have played a pivotal role early metabolic processes biopolymer evolution on prebiotic earth.

Language: Английский

Citations

0
ATP‐Regulated Formation of Transient Peptide Amphiphiles Superstructures DOI Creative Commons
David Cappelletti, Federico Lancia, Andrea Basagni

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 25, 2025

Abstract Self‐assembly of biotic systems serves as inspiration for the preparation synthetic supramolecular assemblies to mimic structural, temporal, and functional aspects living systems. Despite peptide amphiphiles (PAs) being widely studied in context biomimetic bioactive nanomaterials, very little is currently known about reversible spatiotemporal control their hierarchical self‐assemblies. Here, it shown that PA‐based nanofibers can transiently form superstructures, through binding with oppositely charged adenosine triphosphate (ATP), leading charge screening stabilization bundled nanofibers. Enzymatic hydrolysis ATP monophosphate phosphates causes disassembly superstructures recovery individual The lifetime be controlled by adjusting concentration either or enzyme. role formation PA has on chemical reactivity catalysis also evaluated. It observed superstructuration responsible downregulation activity, which then recovered gradual bundles. These results demonstrate potential self‐assembly modulate nanostructures.

Language: Английский

Citations

0
Supramolecular Systems Chemistry Based on the Interplay between Peptides and Porphyrins DOI
Yue Fu, Lian Zhang, Xuehai Yan

et al.

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

Published: Oct. 23, 2024

Abstract The functions of living organisms are emergent from networks biomolecules. In this review, we discuss the creation synthetic life‐like systems based on interplay peptides and porphyrins in supramolecular chemical systems. particular, focus spatiotemporal control self‐assembly processes, which allows for development hierarchical structures biomimetic catalysis adaptive dynamics stimulus‐responsive structural transformations. Notably, when operating a nonequilibrium regime–characterized by kinetic traps, feedback loops, dissipative conditions–the landscape expands system‐level properties emerge, including transient catalysis, metabolic self‐replication, Darwinian‐like evolution. Controlling these at biointerface would facilitate intelligent therapeutic interventions anti‐tumor phototherapy. Supramolecular chemistry provides valuable framework exploring new physicochemical spaces porphyrins, may offer distinct advantages extensive applications across diverse fields.

Language: Английский

Citations

1
Fuel‐driven π‐conjugated Superstructures to Form Transient Conductive Hydrogels DOI
Ifigeneia Tsironi, Jarek A. Maleszka,

Brigitte A. K. Kriebish

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 21, 2024

Abstract Despite advances in creating dissipative materials with transient properties, such as hydrogels and active droplets, their application remains confined to temporal changes structural properties. Developing out‐of‐equilibrium whose electronic functions are parameterized by a chemical reaction cycle is challenging. Yet, this class of required construct biomimetic materials. In contrast traditional cycles that exploit molecularly dissolved building blocks at thermodynamic equilibrium, we show fiber structures derived from reactive naphthalene diimide (NDI) can be used resting states form far‐from‐equilibrium conductive after the addition fuels. Upon fueling NDI‐derived fibers, dual‐component activation deactivation pathway deduced kinetic analysis absent when using state. Investigating solid‐state morphologies formed throughout fuel‐driven cryo‐EM reveals fibers evolve thicker fibrils layered superstructures. We redox‐active exhibit nearly threefold increase electrical conductivity upon fuel consumption before reverting original value over hours. These potential candidates applications programmable biorobotics computing.

Language: Английский

Citations

0