Insights from an information thermodynamics analysis of a synthetic molecular motor

Nature Chemistry, Год журнала: 2022, Номер 14(5), С. 530 - 537

Опубликована: Март 17, 2022

Язык: Английский

---

Non-equilibrium Steady States in Catalysis, Molecular Motors, and Supramolecular Materials: Why Networks and Language Matter

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(26), С. 14169 - 14183

Опубликована: Июнь 21, 2023

All chemists are familiar with the idea that, at equilibrium steady state, relative concentrations of species present in a system predicted by corresponding constants, which related to free energy differences between components. There is also no net flux species, matter how complicated reaction network. Achieving and harnessing non-equilibrium states, coupling network second spontaneous chemical process, has been subject work several disciplines, including operation molecular motors, assembly supramolecular materials, strategies enantioselective catalysis. We juxtapose these linked fields highlight their common features challenges as well some misconceptions that may be serving stymie progress.

Язык: Английский

---

Stimulus-Controlled Anion Binding and Transport by Synthetic Receptors

Chemical Reviews, Год журнала: 2023, Номер 123(13), С. 8530 - 8574

Опубликована: Июнь 21, 2023

Anionic species are omnipresent and involved in many important biological processes. A large number of artificial anion receptors has therefore been developed. Some these capable mediating transmembrane transport. However, where transport proteins can respond to stimuli their surroundings, creation synthetic with stimuli-responsive functions poses a major challenge. Herein, we give full overview the stimulus-controlled that have developed thus far, including application membrane In addition potential operation as carriers, use recognition motifs forming responsive membrane-spanning channels is discussed. With this review article, intend increase interest among scientists working on host–guest complexes dynamic functional systems order stimulate further developments.

Язык: Английский

---

Molecular Ratchets and Kinetic Asymmetry: Giving Chemistry Direction

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(23)

Опубликована: Апрель 3, 2024

Abstract Over the last two decades ratchet mechanisms have transformed understanding and design of stochastic molecular systems—biological, chemical physical—in a move away from mechanical macroscopic analogies that dominated thinking regarding dynamics in 1990s early 2000s (e.g. pistons, springs, etc), to more scale‐relevant concepts underpin out‐of‐equilibrium research sciences today. Ratcheting has established nanotechnology as frontier for energy transduction metabolism, enabled reverse engineering biomolecular machinery, delivering insights into how molecules ‘walk’ track‐based synthesisers operate, acceleration reactions enables be transduced by catalysts (both motor proteins synthetic catalysts), dynamic systems can driven equilibrium through catalysis. The recognition biology, their invention systems, is proving significant areas diverse supramolecular chemistry, covalent DNA nanotechnology, polymer materials science, heterogeneous catalysis, endergonic synthesis, origin life, many other branches science. Put simply, give chemistry direction. Kinetic asymmetry, key feature ratcheting, counterpart structural asymmetry (i.e. chirality). Given ubiquity processes significance behaviour function it surely just fundamentally important. This Review charts recognition, development ratchets, focussing particularly on role which they were originally envisaged elements machinery. Different kinetically asymmetric are compared, consequences discussed. These archetypal examples demonstrate inexorably equilibrium, rather than relax towards it.

Язык: Английский

---

Kinetic Asymmetry and Directionality of Nonequilibrium Molecular Systems

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(9)

Опубликована: Янв. 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.

Язык: Английский

---

Mechanically interlocked [c2]daisy chain backbone enabling advanced shape-memory polymeric materials

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Фев. 24, 2024

Abstract The incorporation of mechanically interlocked structures into polymer backbones has been shown to confer remarkable functionalities materials. In this work, a [ c 2]daisy chain unit based on dibenzo-24-crown-8 is covalently embedded the backbone network, resulting in synthetic material possessing shape-memory properties under thermal control. By decoupling molecular structure three control groups, we demonstrate essential role crosslinks driving shape memory function. topology found be an element for increase glass transition temperature and consequent gain supramolecular host-guest interactions within not only ensure robust mechanical strength good network stability polymer, but also impart with recovery fatigue resistance ability. [c2]daisy as building block potential lay groundwork development wide range

Язык: Английский

---

Is the cell really a machine?

Journal of Theoretical Biology, Год журнала: 2019, Номер 477, С. 108 - 126

Опубликована: Июнь 4, 2019

Язык: Английский

---

Single-molecule FRET methods to study the dynamics of proteins at work

Current Opinion in Biomedical Engineering, Год журнала: 2019, Номер 12, С. 8 - 17

Опубликована: Авг. 23, 2019

Язык: Английский

---

Synthetic Systems Powered by Biological Molecular Motors

Chemical Reviews, Год журнала: 2019, Номер 120(1), С. 288 - 309

Опубликована: Сен. 11, 2019

Biological molecular motors (or biomolecular for short) are nature's solution to the efficient conversion of chemical energy mechanical movement. In biological systems, these fascinating molecules responsible movement molecules, organelles, cells, and whole animals. engineered can potentially be used power actuators engines, shuttle cargo sensors, enable new computing paradigms. Here, we review progress in past decade integration into hybrid nanosystems. After briefly introducing motor proteins kinesin myosin their associated cytoskeletal filaments, recent work aiming actuators, devices. some creation processing information become intertwined at scale, creating a type "active matter". We discuss efforts optimize performance, construct combining artificial components, contrast with current motors. A recurrent theme was induction utilization collective behavior between motile systems powered by motors, advances. The exertion external control over structures has remained topic many studies describing exciting progress. Finally, limitations challenges construction try ascertain if there theoretical performance limits. Engineering potential yield commercially viable devices, but it also sharpens our understanding design problems solved evolution nature. This increased is valuable synthetic biology medicine.

Язык: Английский

---

Hydrazones as New Molecular Tools

Chem, Год журнала: 2020, Номер 6(9), С. 2162 - 2173

Опубликована: Сен. 1, 2020

Язык: Английский

---