Artificial Homeostasis Systems Based on Feedback Reaction Networks: Design Principles and Future Promises DOI

Vinay Ambekar Ranganath,

Indrajit Maity

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(14)

Published: Jan. 16, 2024

Abstract Feedback‐controlled chemical reaction networks (FCRNs) are indispensable for various biological processes, such as cellular mechanisms, patterns, and signaling pathways. Through the intricate interplay of many feedback loops (FLs), FCRNs maintain a stable internal environment. Currently, creating minimalistic synthetic cells is long‐term objective systems chemistry, which motivated by natural integrity. The design, kinetic optimization, analysis to exhibit functions akin those cell still pose significant challenges. Indeed, reaching homeostasis essential engineering components. However, maintaining in artificial against agitations difficult task. Several events can provide us with guidelines conceptual understanding homeostasis, be further applicable designing systems. In this regard, we organize our review driven at different length scales, including homogeneous, compartmentalized, soft material First, stretch quick overview molecular supramolecular systems, toolbox nonlinear homeostatic Moreover, existing history their advanced self‐correcting, regulating properties also emphasized.

Language: Английский

The Future of Molecular Machines DOI Creative Commons
Ivan Aprahamian

ACS Central Science, Journal Year: 2020, Volume and Issue: 6(3), P. 347 - 358

Published: March 3, 2020

Artificial molecular machines have captured the imagination of scientists and nonscientists alike for decades now, given their clear potential to transform enhance all aspects human life. In this Outlook, I use a bicycle as an analogy explain what machine is, in my opinion, work through representative selection case studies specify significant accomplishments made date, obstacles that currently stand between these field's fulfillment its great potential. The hope intentionally sober account is sketch path toward rich exciting research trajectory might challenge current practitioners attract junior into fold. Considering progress we witnessed past decade, am positive future field rosy one.

Language: Английский

Citations

342
Chemically Fueled Self‐Assembly in Biology and Chemistry DOI Creative Commons
Krishnendu Das, Luca Gabrielli, Leonard J. Prins

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(37), P. 20120 - 20143

Published: March 11, 2021

Life is a non-equilibrium state of matter maintained at the expense energy. Nature uses predominantly chemical energy stored in thermodynamically activated, but kinetically stable, molecules. These high-energy molecules are exploited for synthesis other biomolecules, activation biological machinery such as pumps and motors, maintenance structural order. Knowledge how transferred to biochemical processes essential development artificial systems with life-like processes. Here, we discuss can be used control organization organic Four different strategies have been identified according distinguishable physical-organic basis. For each class, one example from biology chemistry discussed detail illustrate practical implementation concept distinct opportunities they offer. Specific attention paid discussion chemically fueled self-assembly. We meaning self-assembly, its kinetic origin, develop synthetic systems.

Language: Английский

Citations

262
New horizons for catalysis disclosed by supramolecular chemistry DOI
Giorgio Olivo, Giorgio Capocasa, Daniele Del Giudice

et al.

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(13), P. 7681 - 7724

Published: Jan. 1, 2021

Recent advancements in supramolecular catalysis are reviewed, which show the potential of related tools when applied to organic synthesis. Such recognized as innovative instruments that can pave way alternative synthetic strategies.

Language: Английский

Citations

150
Chemical fuels for molecular machinery DOI
Stefan Borsley, David A. Leigh, Benjamin M. W. Roberts

et al.

Nature Chemistry, Journal Year: 2022, Volume and Issue: 14(7), P. 728 - 738

Published: July 1, 2022

Language: Английский

Citations

116
Chemical engines: driving systems away from equilibrium through catalyst reaction cycles DOI
Shuntaro Amano, Stefan Borsley, David A. Leigh

et al.

Nature Nanotechnology, Journal Year: 2021, Volume and Issue: 16(10), P. 1057 - 1067

Published: Oct. 1, 2021

Language: Английский

Citations

110
Non-equilibrium Steady States in Catalysis, Molecular Motors, and Supramolecular Materials: Why Networks and Language Matter DOI Creative Commons
Ivan Aprahamian, Stephen M. Goldup

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(26), P. 14169 - 14183

Published: June 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.

Language: Английский

Citations

81
Autonomous Soft Robots Empowered by Chemical Reaction Networks DOI Creative Commons
Giorgio Fusi, Daniele Del Giudice, Oliver Skarsetz

et al.

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(7)

Published: Nov. 24, 2022

Hydrogel actuators are important for designing stimuli-sensitive soft robots. They generate mechanical motion by exploiting compartmentalized (de)swelling in response to a stimulus. However, classical switching methods, such as manually lowering or increasing the pH, cannot provide more complex autonomous motions. By coupling an autonomously operating pH-flip with programmable lifetimes hydrogel system containing pH-responsive and non-responsive compartments, autoonenomous forward backward well tasks, interlocking of "puzzle pieces" collection objects realized. All operations initiated one simple trigger, devices operate "fire forget" mode. More self-regulatory behavior is obtained adding chemo-mechano-chemo feedback mechanisms. Due its simplicity, this method shows great potential operation grippers metamaterials.

Language: Английский

Citations

80
Molecular Ratchets and Kinetic Asymmetry: Giving Chemistry Direction DOI Creative Commons
Stefan Borsley, David A. Leigh, Benjamin M. W. Roberts

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(23)

Published: April 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.

Language: Английский

Citations

40
A Doubly Kinetically-Gated Information Ratchet Autonomously Driven by Carbodiimide Hydration DOI
Stefan Borsley, David A. Leigh, Benjamin M. W. Roberts

et al.

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 143(11), P. 4414 - 4420

Published: March 11, 2021

We report a rotaxane-based information ratchet in which the macrocycle distribution is pumped away from equilibrium using carbodiimide fuel. A carboxylate group on axle, nonequidistant between two binding sites, efficiently catalyzes hydration of fuel to corresponding urea waste, with >80% molecules reacting through machine-catalyzed pathway. The energy reaction harnessed by kinetic differentiation mechanical states machine driving site distal catalyst. Steric hindrance and slows (to form barrier movement) proximal co-conformer, whereas hydrogen bonding accelerates hydrolysis activated ester isomer. directionally biased processes reinforce each other's effect, resulting doubly kinetically gated that achieves 1:18 directionality, an exceptional degree selectivity for synthetic chemically fueled molecular motor.

Language: Английский

Citations

90
Overtemperature-protection intelligent molecular chiroptical photoswitches DOI Creative Commons
Jiabin Yao, Wanhua Wu, Chao Xiao

et al.

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: May 10, 2021

Abstract Stimuli-responsive intelligent molecular machines/devices are of current research interest due to their potential application in minimized devices. Constructing capable accomplishing complex missions is challenging, demanding coalescence various functions into one molecule. Here we report the construction chiroptical photoswitches based on azobenzene-fused bicyclic pillar[ n ]arene derivatives, which defined as universal joints (MUJs). The Z / E photoisomerization azobenzene moiety MUJs induces rolling in/out conformational switching azobenzene-bearing side-ring and consequently leads planar chirality MUJs. Meanwhile, temperature variation was demonstrated also cause conformational/chiroptical inversion significant entropy change during ring-flipping. As a result, photo-induced could be prohibited when exceeded an upper limit, demonstrating photoswitch having over-temperature protection function, stark contrast low-temperature-gating effect commonly encountered.

Language: Английский

Citations

88