scholarly journals Catalytic processing in ruthenium-based polyoxometalate coacervate protocells

2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Pierangelo Gobbo ◽  
Liangfei Tian ◽  
B. V. V. S Pavan Kumar ◽  
Samuel Turvey ◽  
Mattia Cattelan ◽  
...  
Keyword(s):  
Horseradish Peroxidase ◽  
Functional Activity ◽  
Soft Matter ◽  
Collective Behaviour ◽  
Reaction Networks ◽  
Systems Chemistry ◽  
Chemical Signalling ◽  
Catalytic Processing ◽  
New Type ◽  
Important Milestone

AbstractThe development of programmable microscale materials with cell-like functions, dynamics and collective behaviour is an important milestone in systems chemistry, soft matter bioengineering and synthetic protobiology. Here, polymer/nucleotide coacervate micro-droplets are reconfigured into membrane-bounded polyoxometalate coacervate vesicles (PCVs) in the presence of a bio-inspired Ru-based polyoxometalate catalyst to produce synzyme protocells (Ru4PCVs) with catalase-like activity. We exploit the synthetic protocells for the implementation of multi-compartmentalized cell-like models capable of collective synzyme-mediated buoyancy, parallel catalytic processing in individual horseradish peroxidase-containing Ru4PCVs, and chemical signalling in distributed or encapsulated multi-catalytic protocell communities. Our results highlight a new type of catalytic micro-compartment with multi-functional activity and provide a step towards the development of protocell reaction networks.

Electro-oxidation of phenol on a new type of zeolite/graphite biocomposite electrode with horseradish peroxidase

2007 ◽  
Vol 278 (1-2) ◽  
pp. 47-52 ◽  
Author(s):  
R.H. Carvalho ◽  
F. Lemos ◽  
M.A.N.D.A. Lemos ◽  
J.M.S. Cabral ◽  
F. Ramôa Ribeiro
Keyword(s):  
Horseradish Peroxidase ◽  
New Type ◽  
Electro Oxidation ◽  
Oxidation Of Phenol

scholarly journals Ultrafast photomechanical transduction through thermophoretic implosion

2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Nikita Kavokine ◽  
Shuangyang Zou ◽  
Ruibin Liu ◽  
Antoine Niguès ◽  
Bingsuo Zou ◽  
...  
Keyword(s):  
Soft Matter ◽  
Force Measurements ◽  
Direct Manipulation ◽  
Sound Emission ◽  
Laser Illumination ◽  
Scientific Debate ◽  
Ultrafast Imaging ◽  
Laser Propulsion ◽  
Gravitational Systems ◽  
New Type

AbstractSince the historical experiments of Crookes, the direct manipulation of matter by light has been both a challenge and a source of scientific debate. Here we show that laser illumination allows to displace a vial of nanoparticle solution over centimetre-scale distances. Cantilever-based force measurements show that the movement is due to millisecond-long force spikes, which are synchronised with a sound emission. We observe that the nanoparticles undergo negative thermophoresis, and ultrafast imaging reveals that the force spikes are followed by the explosive growth of a bubble in the solution. We propose a mechanism accounting for the propulsion based on a thermophoretic instability of the nanoparticle cloud, analogous to the Jeans’s instability that occurs in gravitational systems. Our experiments demonstrate a new type of laser propulsion and a remarkably violent actuation of soft matter, reminiscent of the strategy used by certain plants to propel their spores.

scholarly journals Grip on complexity in chemical reaction networks

2017 ◽  
Vol 13 ◽  
pp. 1486-1497 ◽  
Author(s):  
Albert S Y Wong ◽  
Wilhelm T S Huck
Keyword(s):  
Complex Networks ◽  
Chemical Reaction ◽  
Biological Networks ◽  
Chemical Reaction Networks ◽  
Living Systems ◽  
Reaction Networks ◽  
Natural Systems ◽  
Systems Chemistry ◽  
Single Chemical ◽  
And Control

A new discipline of “systems chemistry” is emerging, which aims to capture the complexity observed in natural systems within a synthetic chemical framework. Living systems rely on complex networks of chemical reactions to control the concentration of molecules in space and time. Despite the enormous complexity in biological networks, it is possible to identify network motifs that lead to functional outputs such as bistability or oscillations. To truly understand how living systems function, we need a complete understanding of how chemical reaction networks (CRNs) create function. We propose the development of a bottom-up approach to design and construct CRNs where we can follow the influence of single chemical entities on the properties of the network as a whole. Ultimately, this approach should allow us to not only understand such complex networks but also to guide and control their behavior.

scholarly journals Direct mapping of local director field of nematic liquid crystals at the nanoscale

2015 ◽  
Vol 112 (50) ◽  
pp. 15291-15296 ◽  
Author(s):  
Yu Xia ◽  
Francesca Serra ◽  
Randall D. Kamien ◽  
Kathleen J. Stebe ◽  
Shu Yang
Keyword(s):  
Liquid Crystals ◽  
Soft Matter ◽  
Real Space ◽  
Colloidal Systems ◽  
Director Field ◽  
Silica Surfaces ◽  
Dipole Interactions ◽  
Molecular Ordering ◽  
New Type ◽  
Strong Dipole

Liquid crystals (LCs), owing to their anisotropy in molecular ordering, are of wide interest in both the display industry and soft matter as a route to more sophisticated optical objects, to direct phase separation, and to facilitate colloidal assemblies. However, it remains challenging to directly probe the molecular-scale organization of nonglassy nematic LC molecules without altering the LC directors. We design and synthesize a new type of nematic liquid crystal monomer (LCM) system with strong dipole–dipole interactions, resulting in a stable nematic phase and strong homeotropic anchoring on silica surfaces. Upon photopolymerization, the director field can be faithfully “locked,” allowing for direct visualization of the LC director field and defect structures by scanning electron microscopy (SEM) in real space with 100-nm resolution. Using this technique, we study the nematic textures in more complex LC/colloidal systems and calculate the extrapolation length of the LCM.

From systems biology to systems chemistry: metabolomic procedures enable insight into complex chemical reaction networks in water

RSC Advances ◽  
2014 ◽  
Vol 4 (32) ◽  
pp. 16777 ◽  
Author(s):  
Michaël Méret ◽  
Daniel Kopetzki ◽  
Thomas Degenkolbe ◽  
Sabrina Kleessen ◽  
Zoran Nikoloski ◽  
...  
Keyword(s):  
Systems Biology ◽  
Chemical Reaction ◽  
Chemical Reaction Networks ◽  
Reaction Networks ◽  
Complex Chemical ◽  
Complex Chemical Reaction ◽  
Systems Chemistry ◽  
Insight Into

scholarly journals Darwinian properties and their trade-offs in autocatalytic RNA reaction networks

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Sandeep Ameta ◽  
Simon Arsène ◽  
Sophie Foulon ◽  
Baptiste Saudemont ◽  
Bryce E. Clifton ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Network Topology ◽  
Droplet Microfluidics ◽  
Reaction Networks ◽  
Major Goal ◽  
Systems Chemistry ◽  
Trade Offs ◽  
Chemical States ◽  
The Origin Of Life ◽  
Autocatalytic Networks

AbstractDiscovering autocatalytic chemistries that can evolve is a major goal in systems chemistry and a critical step towards understanding the origin of life. Autocatalytic networks have been discovered in various chemistries, but we lack a general understanding of how network topology controls the Darwinian properties of variation, differential reproduction, and heredity, which are mediated by the chemical composition. Using barcoded sequencing and droplet microfluidics, we establish a landscape of thousands of networks of RNAs that catalyze their own formation from fragments, and derive relationships between network topology and chemical composition. We find that strong variations arise from catalytic innovations perturbing weakly connected networks, and that growth increases with global connectivity. These rules imply trade-offs between reproduction and variation, and between compositional persistence and variation along trajectories of network complexification. Overall, connectivity in reaction networks provides a lever to balance variation (to explore chemical states) with reproduction and heredity (persistence being necessary for selection to act), as required for chemical evolution.

scholarly journals Activated Self-Resolution and Error-Correction in Catalytic Reaction Networks

2021 ◽  
Author(s):  
Fredrik Schaufelberger ◽  
Olof Ramstrom
Keyword(s):  
Dynamic System ◽  
Error Correction ◽  
Small Molecule ◽  
Catalytic Reaction ◽  
Reaction Network ◽  
Reaction Networks ◽  
Complex Reaction ◽  
Catalytic Systems ◽  
Systems Chemistry ◽  
Mbh Reaction

<p>To understand the emergence of function in complex reaction networks is a primary goal of systems chemistry and origin-of-life studies. Especially challenging is the establishment of systems that simultaneously exhibit several functionality parameters that can be independently tuned. In this work, a multifunctional complex reaction network of nucleophilic small molecule catalysts for the Morita-Baylis-Hillman (MBH) reaction is demonstrated. The dynamic system exhibited triggered self-resolution, preferentially amplifying a specific catalyst/product set out of a many potential alternatives. By utilizing selective reversibility of the products of the reaction set, systemic thermodynamically driven error-correction could also be introduced. To achieve this, a dynamic covalent MBH reaction based on adducts with internal H-transfer capabilities was developed, displaying rate accelerations of retro-MBH reactions up to 104 times. This study demonstrates how efficient self-sorting of catalytic systems can be achieved through an interplay of several complex emergent functionalities.</p>

scholarly journals Structure Elucidation of a Cryptic Condensation Product from Diacetyl and Arylamine – Then and Now

2020 ◽  
Vol 74 (4) ◽  
pp. 293-297
Author(s):  
Lukas Hintermann
Keyword(s):  
Structure Elucidation ◽  
Organic Molecules ◽  
Condensation Product ◽  
Real Life ◽  
2D Nmr ◽  
Reaction Networks ◽  
Classical Approach ◽  
Condensation Products ◽  
Nmr Techniques ◽  
New Type

Some 70 years ago, the reaction of diacetyl (1) and arylamines (2) in hot phosphoric acid was reported to give a new type of condensation products, but no structure was assigned to them. The case is presented to recapitulate the methods and rationales used in classical structure elucidation of organic molecules through reaction networks, before spectroscopic or crystallographic methods were generally available. The difficulties and limits of the classical approach are exemplified through this real-life problem, which could not be solved by the methodology of its time. A representative condensation product 4a has been resynthesized from 1 and p-toluidine (2a), and its structure elucidation by means of 2D NMR techniques is outlined. Keywords

scholarly journals Activated Self-Resolution and Error-Correction in Catalytic Reaction Networks

2021 ◽  
Author(s):  
Fredrik Schaufelberger ◽  
Olof Ramstrom
Keyword(s):  
Dynamic System ◽  
Error Correction ◽  
Small Molecule ◽  
Catalytic Reaction ◽  
Reaction Network ◽  
Reaction Networks ◽  
Complex Reaction ◽  
Catalytic Systems ◽  
Systems Chemistry ◽  
Mbh Reaction

<p>To understand the emergence of function in complex reaction networks is a primary goal of systems chemistry and origin-of-life studies. Especially challenging is the establishment of systems that simultaneously exhibit several functionality parameters that can be independently tuned. In this work, a multifunctional complex reaction network of nucleophilic small molecule catalysts for the Morita-Baylis-Hillman (MBH) reaction is demonstrated. The dynamic system exhibited triggered self-resolution, preferentially amplifying a specific catalyst/product set out of a many potential alternatives. By utilizing selective reversibility of the products of the reaction set, systemic thermodynamically driven error-correction could also be introduced. To achieve this, a dynamic covalent MBH reaction based on adducts with internal H-transfer capabilities was developed, displaying rate accelerations of retro-MBH reactions up to 104 times. This study demonstrates how efficient self-sorting of catalytic systems can be achieved through an interplay of several complex emergent functionalities.</p>

scholarly journals Darwinian properties and their trade-offs in autocatalytic RNA reaction networks

2019 ◽  
Author(s):  
Sandeep Ameta ◽  
Simon Arsène ◽  
Sophie Foulon ◽  
Baptiste Saudemont ◽  
Bryce E. Clifton ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Network Topology ◽  
Droplet Microfluidics ◽  
Reaction Networks ◽  
Major Goal ◽  
Systems Chemistry ◽  
Trade Offs ◽  
Chemical States ◽  
The Origin Of Life ◽  
Autocatalytic Networks

Discovering autocatalytic chemistries that can evolve is a major goal in systems chemistry and a critical step towards understanding the origin of life. Autocatalytic networks have been discovered in various chemistries, but we lack a general understanding of how network topology controls the Darwinian properties of variation, differential reproduction, and heredity, which are mediated by the chemical composition. Using barcoded sequencing and droplet microfluidics, we establish a landscape of thousands of networks of RNAs that catalyze their own formation from fragments, and derive relationships between network topology and chemical composition. We find that strong variations arise from catalytic innovations perturbing weakly connected networks, and that reproduction increases with global connectivity. These rules imply trade-offs between reproduction and variation, and between compositional persistence and variation along trajectories of network complexification. Overall, connectivity in reaction networks provides a lever to balance variation (to explore chemical states) with reproduction and heredity (persistence being necessary for selection to act), as required for chemical evolution.

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