Menthyl acetate powered self-propelled Janus sponge Marangoni motors with self-maintaining surface tension gradients and active mixing.

Hypothesis: Small scale Marangoni motors, which self-generate motion by inducing surface tension gradients on water interfaces through release of surface-active "fuels", have recently been proposed as self-powered mixing devices for low volume fluids. Such devices however, often show self-limiting lifespans due to the rapid saturation of surface-active agents. A potential solution to this is the use volatile surface-active agents which do not persist in their environment.

Can self-propelled objects escape from compression stimulation?

We studied circular papers impregnated with camphor (CPs) and CPs with magnets (MCPs) as self-propelled objects floating on water under the compression of the water surface as an inanimate system for evacuation in an emergency. Two water chambers-C and C-were connected a plastic gate, and eight CPs or eight MCPs were placed on C. We monitored the movement of the CPs or MCPs from C to C when the gate was opened and the area of C () was decreased using a barrier.

Effects of the Molecular Structure of Malodor Substances and Their Masking on 1,2-Dioleoyl--glycero-3-phosphocholine Molecular Layers.

Certain odors have been shown not only to cause health problems and stress but also to affect skin barrier function. Therefore, it is important to understand olfactory masking to develop effective fragrances to mask malodors. However, olfaction and olfactory masking mechanisms are not yet fully understood.

Self-propelled motion controlled by ionic liquids.

We studied the self-propulsion of a camphor disk floating on a water surface using two types of ionic liquids (hexylammonium-trifluoroacetate (HHexam-TFA) and hexylethylenediaminium-trifluoroacetate (HHexen-TFA)). Bifurcation between continuous, oscillatory, and no motion was observed depending on the concentration of the ionic liquid. The bifurcation concentration between oscillatory and no motion for HHexam-TFA was lower than that for HHexen-TFA.

Self-propelled object that generates a boundary with amphiphiles at an air/aqueous interface.

A benzoic acid (BA) disk was investigated as a novel self-propelled object whose driving force was the difference in surface tension. 4-Stearoyl amidobenzoic acid (SABA) was synthesized as an amphiphile to control the nature of motion based on intermolecular interactions between BA and SABA. The BA disk exhibited characteristic motion depending on the surface density of the SABA on the aqueous phase, that is, reciprocating motion as a one-dimensional motion and restricted and unrestricted motion as a two-dimensional motion.

Proficiently partitioning of bioactive peptide-ssDNA conjugates by microbead-assisted capillary electrophoresis (MACE).

Low-molecular drug discovery using DNA-encoded chemical library (DEL) is a powerful technology, although improving the partitioning efficiency of affinity ligands from DEL remains a challenge. Here, we assessed the usefulness of microbead-assisted capillary electrophoresis (MACE) for partitioning peptide-oligonucleotide conjugates (POCs), in which high selection pressure is applied because of different mobility of target-modified beads and POCs during CE. Despite their different charge characteristics, all POCs were well separated from the beads.

Phospholipid Molecular Layer that Enhances Distinction of Odors Based on Artificial Sniffing.

We propose a novel odor-sensing system based on the dynamic response of phospholipid molecular layers for artificial olfaction. Organisms obtain information about their surroundings based on multidimensional information obtained from sniffing, i.e.

Oscillatory Motion of an Organic Droplet Reflecting a Reaction Scheme.

An organic droplet containing thymol acetate (TA) floating on a sodium dodecyl sulfate aqueous phase was examined to develop a novel self-propelled object based on reaction kinetics. Two types of oscillatory motion, without back-and-forth motion (Osc I) and with back-and-forth motion (Osc II), were observed by varying the pH of the aqueous phase. The oscillation frequency reached its maximum at pH 9.

Height-dependent oscillatory motion of a plastic cup with a camphor disk floated on water.

We have developed a self-propelled object, which is composed of a plastic cup and a camphor disk, on water to reflect its three-dimensional shape in the nature of motion. The self-propelled object, of which the driving force of motion is the difference in the surface tension, exhibited oscillatory motion between motion and rest. The period and the maximum speed of oscillatory motion increased and decreased depending on the height of the cup, , respectively.

Characteristic growth of chemical gardens from mixtures of two salts.

Chemical gardens formed from two metal salts (MCl or MSO) have been investigated to understand the effects of mixing on the growth of precipitate tubes. The growth of tubes can be classified into three types, , collaborative, inhibited, and individual growth, depending on the combination of the two metal salts. Characteristic features of tube growth are discussed in relation to the flow near the tip of the tube controlled by osmotic pressure and the solubility product, , for M(OH).

Recursively positive and negative chemotaxis coupling with reaction kinetics in self-organized inanimate motion.

Reconstructing recursive chemotaxis in inanimate self-propelled objects is inevitable in the development of recursively and autonomously artificial mass transport systems. However, the fabrication of inanimately recursive chemotaxis has been extremely challenging because of the difficulty in introducing competitive positive and negative feedback into an inanimate self-propelled object. Herein, a coumarin derivative (coumarin, 4-methylcoumarin (4-MC), or 6-methylcoumarin (6-MC))-based disk floated on water as a self-propelled object exhibited characteristic features of motion; these features include continuous motion, repetition between positive and negative chemotaxis to the NaPO powder as a base stimulus, and oscillatory motion above the NaPO powder depending on the NaPO density of the powder and the functional group of coumarin derivatives.

Sequentially Selective Coalescence of Binary Self-Propelled Droplets upon Collective Motion.

Subsequent synthesis and detection using droplets as microreactors have shown promise in the development of novel materials and drugs because microreactors enable small-scale synthesis and detection of covalent/non-covalent intermolecular interactions. Self-organization exhibited by autonomous droplets under non-equilibrium conditions is beneficial for manipulating the sequentiality and selectivity of droplet coalescence because expensive equipment or elaborate techniques are not required with the autonomy of droplets. However, to our knowledge, selective coalescence caused by the collective motion of self-propelled droplets has not been demonstrated in inanimate systems.

Evolution of Proliferative Model Protocells Highly Responsive to the Environment.

In this review, we discuss various methods of reproducing life dynamics using a constructive approach. An increase in the structural complexity of a model protocell is accompanied by an increase in the stage of reproduction of a compartment (giant vesicle; GV) from simple reproduction to linked reproduction with the replication of information molecules (DNA), and eventually to recursive proliferation of a model protocell. An encounter between a plural protic catalyst () and DNA within a GV membrane containing a plural cationic lipid () spontaneously forms a supramolecular catalyst () that catalyzes the production of cationic membrane lipid .

Colocalization Analysis of Lipo-Deoxyribozyme Consisting of DNA and Protic Catalysts in a Vesicle-Based Protocellular Membrane Investigated by Confocal Microscopy.

The linkage between the self-reproduction of compartments and the replication of DNA in a compartment is a crucial requirement for cellular life. In our giant vesicle (GV)-based model protocell, this linkage is achieved through the action of a supramolecular catalyst composed of membrane-intruded DNA and amphiphilic acid catalysts () in a GV membrane. In this study, we examined colocalization analysis for the formation of the supramolecular catalyst using a confocal laser scanning fluorescence microscope with high sensitivity and resolution.

Self-Propelled Motion Sensitive to the Chemical Structure of Amphiphilic Molecular Layer on an Aqueous Phase.

Two novel amphiphiles, -(3-nitrophenyl)stearamide (MANA) and ,-(4-nitro-1,3-phenylene)distearamide (OPANA), were synthesized by reacting nitroanilines with one or two equivalents of stearic acid. We investigated how the molecular structures of these compounds influenced the characteristics of a self-propelled camphor disk placed on a monolayer of the synthesized amphiphiles. Three types of motion were observed at different surface pressures (): continuous motion ( < 4 mN m), deceleration (4 mN ≤ ≤ 20 mN m), and no motion ( > 20 mN m).

Proliferating coacervate droplets as the missing link between chemistry and biology in the origins of life.

The hypothesis that prebiotic molecules were transformed into polymers that evolved into proliferating molecular assemblages and eventually a primitive cell was first proposed about 100 years ago. To the best of our knowledge, however, no model of a proliferating prebiotic system has yet been realised because different conditions are required for polymer generation and self-assembly. In this study, we identify conditions suitable for concurrent peptide generation and self-assembly, and we show how a proliferating peptide-based droplet could be created by using synthesised amino acid thioesters as prebiotic monomers.

Alternate Route Selection of Self-Propelled Filter Papers Impregnated with Camphor for Two-Branched Water Channels.

The route selection of self-propelled filter papers impregnated with camphor for two-branched water channels was investigated. The two-branched water channel was composed of a stem channel and two branch channels, and the branch channels were connected to the stem channel at a junction. When a single camphor paper reached the junction from the stem channel, it selected one of the two routes equivalently.

Environment-Sensitive Intelligent Self-Reproducing Artificial Cell with a Modification-Active Lipo-Deoxyribozyme.

As a supramolecular micromachine with information flow, a giant vesicle (GV)-based artificial cell that exhibits a linked proliferation between GV reproduction and internal DNA amplification has been explored in this study. The linked proliferation is controlled by a complex consisting of GV membrane-intruded DNA with acidic amphiphilic catalysts, working overall as a lipo-deoxyribozyme. Here, we investigated how a GV-based artificial cell containing this lipo-deoxyribozyme responds to diverse external and internal environments, changing its proliferative dynamics.

DNA Length-dependent Division of a Giant Vesicle-based Model Protocell.

DNA is an essential carrier of sequence-based genetic information for all life today. However, the chemical and physical properties of DNA may also affect the structure and dynamics of a vesicle-based model protocell in which it is encapsulated. To test these effects, we constructed a polyethylene glycol-grafted giant vesicle system capable of undergoing growth and division.

A sustainable self-reproducing liposome consisting of a synthetic phospholipid.

A novel phosphoric membrane lipid (phospholipid) bearing an oleyl group as one of the hydrophobic chains formed a liposome with a thin lamella in water. Since the anionic membrane of pre-existing liposomes acted as a catalytic surface in phosphate buffer, membrane lipids could be generated from their precursor in an autocatalytic manner without the inclusion of catalytic amphiphiles in the liposome. The morphological changes of this anionic liposome were monitored both by flow cytometry and optical microscopy, and it was found that the liposomes deformed into a budding shape, followed by division, after the addition of a membrane precursor.

Synthetic Approach to biomolecular science by cyborg supramolecular chemistry.

Background: To imitate the essence of living systems via synthetic chemistry approaches has been attempted. With the progress in supramolecular chemistry, it has become possible to synthesize molecules of a size and complexity close to those of biomacromolecules. Recently, the combination of precisely designed supramolecules with biomolecules has generated structural platforms for designing and creating unique molecular systems.

A recursive vesicle-based model protocell with a primitive model cell cycle.

Self-organized lipid structures (protocells) have been proposed as an intermediate between nonliving material and cellular life. Synthetic production of model protocells can demonstrate the potential processes by which living cells first arose. While we have previously described a giant vesicle (GV)-based model protocell in which amplification of DNA was linked to self-reproduction, the ability of a protocell to recursively self-proliferate for multiple generations has not been demonstrated.