Chem, Journal Year: 2024, Volume and Issue: unknown
Published: Nov. 1, 2024
Language: Английский
Nature Chemistry, Journal Year: 2024, Volume and Issue: 16(9), P. 1558 - 1564
Published: June 10, 2024
Abstract Maxwell’s demon describes a thought experiment in which ‘demon’ regulates the flow of particles between two adjoining spaces, establishing potential gradient without appearing to do work. This seeming paradox led understanding that sorting entails thermodynamic work, foundational concept information theory. In past centuries, many systems analogous have been introduced form molecular information, pumps and ratchets. Here we report functional example material over centimetres, whereas previous examples operated on scale. our system, this drives directional transport o -fluoroazobenzene arms U-tube apparatus upon light irradiation, transiting through an aqueous membrane containing coordination cage. The concentration thus obtained is further harnessed drive naphthalene opposite direction.
Language: Английский
Citations
5
Chem, Journal Year: 2023, Volume and Issue: 10(4), P. 1147 - 1159
Published: Dec. 29, 2023
Language: Английский
Citations
12
ACS Nano, Journal Year: 2024, Volume and Issue: 18(18), P. 11898 - 11909
Published: April 22, 2024
Electrochemical liquid electron microscopy has revolutionized our understanding of nanomaterial dynamics by allowing for direct observation their electrochemical production. This technique, primarily applied to inorganic materials, is now being used explore the self-assembly active molecular materials. Our study examines these across various scales, from nanoscale behavior individual fibers micrometer-scale hierarchical evolution fiber clusters. To isolate influences beam and electrical potential on material behavior, we conducted thorough beam–sample interaction analyses. findings reveal that materials at are shaped proximity electrode current. By integrating observations with reaction–diffusion simulations, uncover local structures formation history play a crucial role in determining assembly rates. suggests emergence nonequilibrium can locally accelerate further structural development, offering insights into under conditions.
Language: Английский
Citations
4
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 64(2)
Published: Aug. 17, 2024
Biomolecular machines autonomously convert energy into functions, driving systems away from thermodynamic equilibrium. This conversion is achieved by leveraging complex, kinetically asymmetric chemical reaction networks that are challenging to characterize precisely. In contrast, all known synthetic molecular in which kinetic asymmetry has been quantified well described simple single-cycle networks. Here, we report on a unique light-driven [2]rotaxane enables the autonomous operation of machine with multi-cycle network. Unlike prior systems, present one exploits photoactive macrocycle, features different photoreactivity depending binding sites at it resides. Furthermore, E Z isomerization reverses relative affinity macrocycle for two axle, resulting Building most recent theoretical advancements, this work quantifies network first time. Our findings represent simplest rotaxane capable shuttling developed so far and offer general strategy generate quantify beyond systems.
Language: Английский
Citations
4
Colloids and Interface Science Communications, Journal Year: 2025, Volume and Issue: 66, P. 100829 - 100829
Published: March 21, 2025
Language: Английский
Citations
0
Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown
Published: May 9, 2025
Abstract Living systems adapt to mechanical forces through a series of biochemical feedback loops and dissipative signal transduction mechanisms across multiple length scales. By contrast, synthetic materials are static, closed with minimal interaction their surroundings lack the ability deformations. Here, strategy that enables hydrogel temporal modulation its stiffness properties is reported. It demonstrated force‐induced bond rupture at disulfide linkages hydrogel, coupled chemical reoxidation leads dissipative, transient functions. The electrochemical generation oxidant as output loop triggered by an externally applied force provides high spatiotemporal control over process, enabling engineering hydrogels out‐of‐equilibrium patterns. Additionally, dose‐controlled, release model protein payloads from demonstrated. proposed concept has potential enhance autonomous interactive functionalities hydrogels, advancing applications in biomedical field soft robotics.
Language: Английский
Citations
0
Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(9)
Published: Jan. 18, 2024
Abstract Scientists have long been fascinated by the biomolecular machines in living systems that process energy and information to sustain life. The first synthetic molecular rotor capable of performing repeated 360° rotations due a combination photo‐ thermally activated processes was reported 1999. progress designing different intervening years has remarkable, with several outstanding examples appearing last few years. Despite accomplishments, there remains confusion regarding fundamental design principles which motions molecules can be controlled, significant intellectual tension between mechanical chemical ways thinking about describing machines. A thermodynamically consistent analysis kinetics rotors pumps shows while light driven operate power‐stroke mechanism, kinetic asymmetry—the relative heights barriers—is sole determinant directionality catalysis Power‐strokes—the depths wells—play no role whatsoever determining sign directionality. These results, elaborated using trajectory thermodynamics nonequilibrium pump equality, show asymmetry governs response many non‐equilibrium phenomena.
Language: Английский
Citations
3
Chemistry - A European Journal, Journal Year: 2024, Volume and Issue: 30(37)
Published: April 8, 2024
A well-behaved dynamic library composed of two imines and corresponding amines was subjected to the action an activated carboxylic acid (ACA), whose decarboxylation is known be base promoted, in different solvents, namely CD
Language: Английский
Citations
3
Angewandte Chemie, Journal Year: 2023, Volume and Issue: 135(47)
Published: Aug. 7, 2023
Abstract Non‐equilibrium chemical systems underpin multiple domains of contemporary interest, including supramolecular chemistry, molecular machines, prebiotic and energy transduction. Experimental chemists are now pioneering the realization artificial that can harvest away from equilibrium. In this tutorial Review, we provide an overview ratchets: mechanisms enabling absorption environment. By focusing on mechanism type—rather than application domain or source—we offer a unifying picture seemingly disparate phenomena, which hope will foster progress in fascinating science.
Language: Английский
Citations
6
Chemistry - A European Journal, Journal Year: 2023, Volume and Issue: 29(40)
Published: May 10, 2023
Benefiting from the features like polymeric linear structures, stimuli-responsiveness and dynamic adaptiveness, supramolecular polymers (SPs) are favored as exploiting muscle-like materials, allowing for imitating muscle functions. However, a substantial part of these materials barely owned an unitary motion orientation while it was obviously known that movements involved distinct orientations. Herein, M1 holding structure 44-membered macrocycle with two aldehyde groups designed, meanwhile, M2 comprising secondary ammonium ions, 3,5-di-tert-butylphenyl well alkyl chains fabricated, which could be assembled to generate SPs based on host-guest interactions large ions. underwent vertical compression upon addition N2 H4 owing forming covalent bonds, notably, mechanically interlocked structures were also generated. Afterwards, vertically compressed experienced horizontal shrinkage when tetrabutylammonium chloride contributed due destruction interactions.
Language: Английский
Citations
4