scholarly journals Spontaneous formation of autocatalytic sets with self-replicating inorganic metal oxide clusters

2020 ◽  
Vol 117 (20) ◽  
pp. 10699-10705 ◽  
Author(s):  
Haralampos N. Miras ◽  
Cole Mathis ◽  
Weimin Xuan ◽  
De-Liang Long ◽  
Robert Pow ◽  
...  
Keyword(s):  
Molecular Recognition ◽  
Inorganic Salt ◽  
Molybdenum Blue ◽  
Keggin Ion ◽  
Metal Oxide Clusters ◽  
Spontaneous Formation ◽  
Autocatalytic Sets ◽  
Kinetic Investigations ◽  
Inorganic Molecules ◽  
Small Clusters

Here we show how a simple inorganic salt can spontaneously form autocatalytic sets of replicating inorganic molecules that work via molecular recognition based on the {PMo12} ≡ [PMo12O40]3– Keggin ion, and {Mo36} ≡ [H3Mo57M6(NO)6O183(H2O)18]22– cluster. These small clusters are able to catalyze their own formation via an autocatalytic network, which subsequently template the assembly of gigantic molybdenum-blue wheel {Mo154} ≡ [Mo154O462H14(H2O)70]14–, {Mo132} ≡ [MoVI72MoV60O372(CH3COO)30(H2O)72]42– ball-shaped species containing 154 and 132 molybdenum atoms, and a {PMo12}⊂{Mo124Ce4} ≡ [H16MoVI100MoV24Ce4O376(H2O)56 (PMoVI10MoV2O40)(C6H12N2O4S2)4]5– nanostructure. Kinetic investigations revealed key traits of autocatalytic systems including molecular recognition and kinetic saturation. A stochastic model confirms the presence of an autocatalytic network involving molecular recognition and assembly processes, where the larger clusters are the only products stabilized by the cycle, isolated due to a critical transition in the network.

scholarly journals Spontaneous Formation of Autocatalytic Sets with Self-Replicating Inorganic Metal Oxide Clusters

2019 ◽  
Author(s):  
Haralampos N. Miras ◽  
Cole Mathis ◽  
Weimin Xuan ◽  
De-Liang Long ◽  
Robert Pow ◽  
...  
Keyword(s):  
Molecular Recognition ◽  
Fundamental Problem ◽  
Sequence Information ◽  
Formation Kinetic ◽  
Molybdenum Blue ◽  
Autocatalytic Sets ◽  
Kinetic Investigations ◽  
Inorganic Molecules ◽  
Small Clusters ◽  
Self Replication

Biological self-replication is driven by complex machinery requiring large amounts of sequence information too complex to have formed spontaneously. This presents a fundamental problem for understanding the origins self-replication and by extension, life. One route for the emergence of self-replicators is via autocatalytic sets, but experimentally these have been based on RNA and require sequence information. Showing an example outside of biology, would give insights into how the universal ‘life-like’ chemistry can be. Here we show how a simple inorganic salt can spontaneously form information-rich, autocatalytic sets of replicating inorganic molecules that work via molecular recognition based on the {PMo12} Keggin ion, and {Mo36} cluster. These small clusters are involved in an autocatalytic network, where the assembly of gigantic molybdenum blue wheel (Mo154-blue), {Mo132} ball containing 154 and 132 molybdenum atoms, and a new {PMo12}Ì{Mo124 Ce4} nanostructure are templated by the smaller clusters which are themselves able to catalyse their own formation. Kinetic investigations revealed key traits of autocatalytic systems including molecular recognition and kinetic saturation. A stochastic model confirms the presence of an autocatalytic network driven by molecular recognition, where the larger clusters are the only products stabilised by information contained in the cycle, isolated due to a critical transition in the network. This study demonstrates how information-rich autocatalytic sets, based on simple inorganic salts, can spontaneously emerge which are capable of collective self-reproduction outside of biology.<br>

scholarly journals Spontaneous Formation of Autocatalytic Sets with Self-Replicating Inorganic Metal Oxide Clusters

2019 ◽  
Author(s):  
Haralampos N. Miras ◽  
Cole Mathis ◽  
Weimin Xuan ◽  
De-Liang Long ◽  
Robert Pow ◽  
...  
Keyword(s):  
Molecular Recognition ◽  
Fundamental Problem ◽  
Sequence Information ◽  
Formation Kinetic ◽  
Molybdenum Blue ◽  
Autocatalytic Sets ◽  
Kinetic Investigations ◽  
Inorganic Molecules ◽  
Small Clusters ◽  
Self Replication

Biological self-replication is driven by complex machinery requiring large amounts of sequence information too complex to have formed spontaneously. This presents a fundamental problem for understanding the origins self-replication and by extension, life. One route for the emergence of self-replicators is via autocatalytic sets, but experimentally these have been based on RNA and require sequence information. Showing an example outside of biology, would give insights into how the universal ‘life-like’ chemistry can be. Here we show how a simple inorganic salt can spontaneously form information-rich, autocatalytic sets of replicating inorganic molecules that work via molecular recognition based on the {PMo12} Keggin ion, and {Mo36} cluster. These small clusters are involved in an autocatalytic network, where the assembly of gigantic molybdenum blue wheel (Mo154-blue), {Mo132} ball containing 154 and 132 molybdenum atoms, and a new {PMo12}Ì{Mo124 Ce4} nanostructure are templated by the smaller clusters which are themselves able to catalyse their own formation. Kinetic investigations revealed key traits of autocatalytic systems including molecular recognition and kinetic saturation. A stochastic model confirms the presence of an autocatalytic network driven by molecular recognition, where the larger clusters are the only products stabilised by information contained in the cycle, isolated due to a critical transition in the network. This study demonstrates how information-rich autocatalytic sets, based on simple inorganic salts, can spontaneously emerge which are capable of collective self-reproduction outside of biology.<br>

scholarly journals The macroscopic shape of assemblies formed from microparticles based on host–guest interaction dependent on the guest content

2021 ◽  
Vol 11 (1) ◽  
Author(s):  
Takahiro Itami ◽  
Akihito Hashidzume ◽  
Yuri Kamon ◽  
Hiroyasu Yamaguchi ◽  
Akira Harada
Keyword(s):  
Molecular Recognition ◽  
Smart Materials ◽  
Self Assembly ◽  
Early Stage ◽  
Contact Point ◽  
Sodium Acrylate ◽  
Contact Points ◽  
Assembly Behavior ◽  
Small Clusters ◽  
Macroscopic Shape

AbstractBiological macroscopic assemblies have inspired researchers to utilize molecular recognition to develop smart materials in these decades. Recently, macroscopic self-assemblies based on molecular recognition have been realized using millimeter-scale hydrogel pieces possessing molecular recognition moieties. During the study on macroscopic self-assembly based on molecular recognition, we noticed that the shape of assemblies might be dependent on the host–guest pair. In this study, we were thus motivated to study the macroscopic shape of assemblies formed through host–guest interaction. We modified crosslinked poly(sodium acrylate) microparticles, i.e., superabsorbent polymer (SAP) microparticles, with β-cyclodextrin (βCD) and adamantyl (Ad) residues (βCD(x)-SAP and Ad(y)-SAP microparticles, respectively, where x and y denote the mol% contents of βCD and Ad residues). Then, we studied the self-assembly behavior of βCD(x)-SAP and Ad(y)-SAP microparticles through the complexation of βCD with Ad residues. There was a threshold of the βCD content in βCD(x)-SAP microparticles for assembly formation between x = 22.3 and 26.7. On the other hand, the shape of assemblies was dependent on the Ad content, y; More elongated assemblies were formed at a higher y. This may be because, at a higher y, small clusters formed in an early stage can stick together even upon collisions at a single contact point to form elongated aggregates, whereas, at a smaller y, small clusters stick together only upon collisions at multiple contact points to give rather circular assemblies. On the basis of these observations, the shape of assembly formed from microparticles can be controlled by varying y.

scholarly journals Control of the macroscopic shape of assemblies formed from microparticles based on host–guest interaction

2020 ◽  
Author(s):  
Takahiro Itami ◽  
Akihito Hashidzume ◽  
Yuri Kamon ◽  
Hiroyasu Yamaguchi ◽  
Akira Harada
Keyword(s):  
Molecular Recognition ◽  
Smart Materials ◽  
Self Assembly ◽  
Early Stage ◽  
Contact Point ◽  
Sodium Acrylate ◽  
Contact Points ◽  
Assembly Behavior ◽  
Small Clusters ◽  
Macroscopic Shape

Abstract Biological macroscopic assemblies have inspired researchers to utilize molecular recognition to develop smart materials in these decades. Recently, macroscopic self-assemblies based on molecular recognition have been realized using millimeter-scale hydrogel pieces possessing molecular recognition moieties. During the study on macroscopic self-assembly based on molecular recognition, we noticed that the shape of assemblies might be dependent on the host–guest pair. In this study, we were thus motivated to study the macroscopic shape of assemblies formed through host–guest interaction. We modified crosslinked poly(sodium acrylate) microparticles, i.e., superabsorbent polymer (SAP) microparticles, with β-cyclodextrin (βCD) and adamantyl (Ad) residues (βCD(x)-SAP and Ad(y)-SAP microparticles, respectively, where x and y denote the mol % contents of βCD and Ad residues). Then, we studied the self-assembly behavior of βCD(x)-SAP and Ad(y)-SAP microparticles through the complexation of βCD with Ad residues. There was a threshold of the βCD content in βCD(x)-SAP microparticles for assembly formation between x = 22.3 and 26.7. On the other hand, the shape of assemblies was dependent on the Ad content, y; More elongated assemblies were formed at a higher y. This may be because, at a higher y, small clusters formed in an early stage can stick together even upon collisions at a single contact point to form elongated aggregates, whereas, at a smaller y, small clusters stick together only upon collisions at multiple contact points to give rather circular assemblies. On the basis of these observations, the shape of assembly formed from microparticles can be controlled by varying y.

scholarly journals Autocatalytic Networks at the Basis of Life’s Origin and Organization

Life ◽  
2018 ◽  
Vol 8 (4) ◽  
pp. 62 ◽  
Author(s):  
Wim Hordijk ◽  
Mike Steel
Keyword(s):  
Sufficient Condition ◽  
Autocatalytic Sets ◽  
Autopoietic Systems ◽  
Mathematical Formalization ◽  
The Origin Of Life ◽  
1960S And 1970S ◽  
The 1960S ◽  
Inorganic Molecules ◽  
Minimal Life ◽  
Autocatalytic Networks

Life is more than the sum of its constituent molecules. Living systems depend on a particular chemical organization, i.e., the ways in which their constituent molecules interact and cooperate with each other through catalyzed chemical reactions. Several abstract models of minimal life, based on this idea of chemical organization and also in the context of the origin of life, were developed independently in the 1960s and 1970s. These models include hypercycles, chemotons, autopoietic systems, (M,R)-systems, and autocatalytic sets. We briefly compare these various models, and then focus more specifically on the concept of autocatalytic sets and their mathematical formalization, RAF theory. We argue that autocatalytic sets are a necessary (although not sufficient) condition for life-like behavior. We then elaborate on the suggestion that simple inorganic molecules like metals and minerals may have been the earliest catalysts in the formation of prebiotic autocatalytic sets, and how RAF theory may also be applied to systems beyond chemistry, such as ecology, economics, and cognition.

scholarly journals The macroscopic shape of assemblies formed from microparticles based on host–guest interaction dependent on the guest content

2020 ◽  
Author(s):  
Takahiro Itami ◽  
Akihito Hashidzume ◽  
Yuri Kamon ◽  
Hiroyasu Yamaguchi ◽  
Akira Harada
Keyword(s):  
Molecular Recognition ◽  
Smart Materials ◽  
Self Assembly ◽  
Early Stage ◽  
Contact Point ◽  
Sodium Acrylate ◽  
Contact Points ◽  
Assembly Behavior ◽  
Small Clusters ◽  
Macroscopic Shape

Abstract Biological macroscopic assemblies have inspired researchers to utilize molecular recognition to develop smart materials in these decades. Recently, macroscopic self-assemblies based on molecular recognition have been realized using millimeter-scale hydrogel pieces possessing molecular recognition moieties. During the study on macroscopic self-assembly based on molecular recognition, we noticed that the shape of assemblies might be dependent on the host–guest pair. In this study, we were thus motivated to study the macroscopic shape of assemblies formed through host–guest interaction. We modified crosslinked poly(sodium acrylate) microparticles, i.e., superabsorbent polymer (SAP) microparticles, with β-cyclodextrin (βCD) and adamantyl (Ad) residues (βCD(x)-SAP and Ad(y)-SAP microparticles, respectively, where x and y denote the mol % contents of βCD and Ad residues). Then, we studied the self-assembly behavior of βCD(x)-SAP and Ad(y)-SAP microparticles through the complexation of βCD with Ad residues. There was a threshold of the βCD content in βCD(x)-SAP microparticles for assembly formation between x = 22.3 and 26.7. On the other hand, the shape of assemblies was dependent on the Ad content, y; More elongated assemblies were formed at a higher y. This may be because, at a higher y, small clusters formed in an early stage can stick together even upon collisions at a single contact point to form elongated aggregates, whereas, at a smaller y, small clusters stick together only upon collisions at multiple contact points to give rather circular assemblies. On the basis of these observations, the shape of assembly formed from microparticles can be controlled by varying y.

The relationship of IGE receptor topography to signaling activity in RBL-2H3 mast cells

1991 ◽  
Vol 49 ◽  
pp. 236-237
Author(s):  
J.R. Pfeiffer ◽  
J.C. Seagrave ◽  
C. Wofsy ◽  
J.M. Oliver
Keyword(s):  
Mast Cells ◽  
Protein A ◽  
Scattered Electron ◽  
Ige Receptor ◽  
Receptor Complexes ◽  
Ige Binding ◽  
Electron Imaging ◽  
Small Clusters ◽  
Relationship Of ◽  
The Relationship

In RBL-2H3 rat leukemic mast cells, crosslinking IgE-receptor complexes with anti-IgE antibody leads to degranulation. Receptor crosslinking also stimulates the redistribution of receptors on the cell surface, a process that can be observed by labeling the anti-IgE with 15 nm protein A-gold particles as described in Stump et al. (1989), followed by back-scattered electron imaging (BEI) in the scanning electron microscope. We report that anti-IgE binding stimulates the redistribution of IgE-receptor complexes at 37“C from a dispersed topography (singlets and doublets; S/D) to distributions dominated sequentially by short chains, small clusters and large aggregates of crosslinked receptors. These patterns can be observed (Figure 1), quantified (Figure 2) and analyzed statistically. Cells incubated with 1 μg/ml anti-IgE, a concentration that stimulates maximum net secretion, redistribute receptors as far as chains and small clusters during a 15 min incubation period. At 3 and 10 μg/ml anti-IgE, net secretion is reduced and the majority of receptors redistribute rapidly into clusters and large aggregates.

Molecular architecture and functions of the neuronal cytoskeleton

1990 ◽  
Vol 48 (3) ◽  
pp. 2-3
Author(s):  
Nobutaka Hirokawa
Keyword(s):  
Major Elements ◽  
Molecular Structures ◽  
Organelle Transport ◽  
Molecular Architecture ◽  
Neuronal Morphogenesis ◽  
Microtubule Associated Proteins ◽  
Associated Proteins ◽  
And Function ◽  
Small Clusters

In this symposium I will present our studies about the molecular architecture and function of the cytomatrix of the nerve cells. The nerve cell is a highly polarized cell composed of highly branched dendrites, cell body, and a single long axon along the direction of the impulse propagation. Each part of the neuron takes characteristic shapes for which the cytoskeleton provides the framework. The neuronal cytoskeletons play important roles on neuronal morphogenesis, organelle transport and the synaptic transmission. In the axon neurofilaments (NF) form dense arrays, while microtubules (MT) are arranged as small clusters among the NFs. On the other hand, MTs are distributed uniformly, whereas NFs tend to run solitarily or form small fascicles in the dendrites Quick freeze deep etch electron microscopy revealed various kinds of strands among MTs, NFs and membranous organelles (MO). These structures form major elements of the cytomatrix in the neuron. To investigate molecular nature and function of these filaments first we studied molecular structures of microtubule associated proteins (MAP1A, MAP1B, MAP2, MAP2C and tau), and microtubules reconstituted from MAPs and tubulin in vitro. These MAPs were all fibrous molecules with different length and formed arm like projections from the microtubule surface.

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