Engineering pH-Responsive, Self-Healing Vesicle-Type Artificial Tissues with Higher-Order Cooperative Functionalities.

Multicellular organisms demonstrate a hierarchical organization where multiple cells collectively form tissues, thereby enabling higher-order cooperative functionalities beyond the capabilities of individual cells. Drawing inspiration from this biological organization, assemblies of multiple protocells are developed to create novel functional materials with emergent higher-order cooperative functionalities. This paper presents new artificial tissues derived from multiple vesicles, which serve as protocellular models. These tissues are formed and manipulated through non-covalent interactions triggered by a salt bridge. Exhibiting pH-sensitive reversible formation and destruction under neutral conditions, these artificial vesicle tissues demonstrate three distinct higher-order cooperative functionalities: transportation of large cargoes, photo-induced contractions, and enhanced survivability against external threats. The rapid assembly and disassembly of these artificial tissues in response to pH variations enable controlled mechanical task performance. Additionally, the self-healing property of these artificial tissues indicates robustness against external mechanical damage. The research suggests that these vesicles can detect specific pH environments and spontaneously assemble into artificial tissues with advanced functionalities. This leads to the possibility of developing intelligent materials with high environmental specificity, particularly for applications in soft robotics.

Comparative investigation of fine bubble and macrobubble aeration on gas utility and biotransformation productivity.

The sufficient provision of oxygen is mandatory for enzymatic oxidations in aqueous solution, however, in process optimization this still is a bottleneck that cannot be overcome with the established methods of macrobubble aeration. Providing higher mass transfer performance through microbubble aerators, inefficient aeration can be overcome or improved. Investigating the mass transport performance in a model protein solution, the microbubble aeration results in higher kL a values related to the applied airstream in comparison with macrobubble aeration. Comparing the aerators at identical kL a of 160 and 60 1/h, the microbubble aeration is resulting in 25 and 44 times enhanced gas utility compared with aeration with macrobubbles. To prove the feasibility of microbubbles in biocatalysis, the productivity of a glucose oxidase catalyzed biotransformation is compared with macrobubble aeration as well as the gas-saving potential. In contrast to the expectation that the same productivities are achieved at identically applied kL a, microbubble aeration increased the gluconic acid productivity by 32% and resulted in 41.6 times higher oxygen utilization. The observed advantages of microbubble aeration are based on the large volume-specific interfacial area combined with a prolonged residence time, which results in a high mass transfer performance, less enzyme deactivation by foam formation, and reduced gas consumption. This makes microbubble aerators favorable for application in biocatalysis.

Microbubble enhanced mass transfer efficiency of CO2 capture utilizing aqueous triethanolamine for enzymatic resorcinol carboxylation.

The present study focuses on the aeration of aqueous triethanolamine acting as reaction medium for biocatalytic carboxylations. For enhancing mass transfer in a bubble column reactor, microbubble aeration is applied and compared to conventional macrobubble aeration. Application of a 0.5 µm porous sparger enables microbubble CO2 aeration with bubble size distributions below 150 µm in Sauter mean diameter, correlating with the highest measured mass transfer rates. During CO2 saturation of the aqueous triethanolamine, bubble size distributions changed according to the level of CO2 saturation. For microbubbles, less foaming was observed compared to macrobubble aeration by a 10 µm porous sparger. This microbubble effect is attributed to their accelerated dissolution assisted by the Laplace pressure lowering the amount of bubbles reaching the surface of the liquid. The experiments reveal that the rate of interfacial area generation, which is calculated based on measured bubble size distributions, influences the biocatalyst activity.

Destabilization of ultrafine bubbles in water using indirect ultrasonic irradiation.

Ultrafine bubble (UFB) is a bubble with a diameter of less than 1 µm. Little attention has been paid to the defoaming and removal of UFBs. This study proposes a method to destabilize UFBs by using indirect ultrasonic irradiation. Besides, the destabilization mechanism of UFB was investigated. The ultrasonic frequency was 1.6 MHz and the dissipated power was 30 W. UFB dispersions were prepared using two different types of bubble generators: pressurized dissolution method and swirling liquid flow method. The effects of ultrasonic irradiation on the stability of UFBs were evaluated by particle tracking analysis (PTA) and electrophoretic zeta potential measurement. Results showed that the indirect ultrasonic irradiation for 30 min reduced the number concentration of UFBs by 90% regardless of the generation method. This destabilization was attributed to a decrease in the magnitude of zeta potential of UFBs due to the changes in pH and electrical conductivity. These changes in the electrochemical properties were caused by the formation of nitric acid. To study the destabilization mechanism, the pH of the UFB dispersions were modified by titration; the chemical and mechanical effects of ultrasound were separately examined. It was found that not only the chemical effect caused by the formation of nitric acid but also the mechanical effect contributed to the destabilization of UFB. Feasibility studies were also performed for UFBs in an aqueous surfactant solution and UFBs in a solid particle dispersion. The proposed method selectively destabilized UFBs in the solutions.

Effect of surfactant addition on removal of microbubbles using ultrasound.

It is difficult to control the bubble in a liquid by the external operation, because the behavior of the bubble is controlled in buoyancy and flow of liquid. On the other hand, microbubbles, whose diameter is several decades µm, stably disperse in static liquid because of their small buoyancy and electrical repulsion. When an ultrasound, whose frequency was 2.4 MHz, was irradiated, the milky white microbubbles suspended solution became rapidly clear. In this study, the effects of surfactant addition on the removal of microbubbles from a liquid in an ultrasonic field were investigated. The efficiency of removal of microbubbles decreased with surfactant addition. Surfactant type influenced the size of agglomerated microbubbles, and the efficiency of removal of microbubbles changed. The surface of microbubble was modified by surfactant adsorption, and the steric inhibition influenced the removal of microbubbles.

Effect of irradiation distance on degradation of phenol using indirect ultrasonic irradiation method.

Ultrasound is used as degradation of hazardous organic compounds. In this study, indirect ultrasonic irradiation method was applied to the degradation process of phenol, the model hazardous organic compound, and the effects of irradiation distance on radical generation and ultrasonic power were investigated. The chemical effect estimated by KI oxidation dosimetry and ultrasonic power measured by calorimetry fluctuated for the irradiation distance, and there was a relationship between the period of the fluctuation of ultrasonic effect and the wavelength of ultrasound. The degradation of phenol was considered to progress in the zero-order kinetics, before the decomposition conversion was less than 25%. Therefore, the simple kinetic model on degradation of phenol was proposed, and there was a linear relation in the degradation rate constant of phenol and the ultrasonic power inside the reactor. In addition, the kinetic model proposed in this study was applied to the former study. There was a linear relation in the degradation rate constant of phenol and ultrasonic energy in the range of frequency of 20-30 kHz in spite of the difference of equipment and sample volume. On the other hand, the degradation rate constant in the range of frequency of 200-800 kHz was much larger than that of 20-30 kHz in the same ultrasonic energy, and this behaviour was agreed with the former investigation about the dependence of ultrasonic frequency on chemical effect.

Agglomeration and rapid ascent of microbubbles by ultrasonic irradiation.

Microbubbles have some different characteristics from conventional bubbles. To apply the useful properties for gas-liquid contact operation in industry, however, a separate technology of microbubbles has to be realized. In this study, promotion of microbubble separation using ultrasound was proposed. By irradiating with ultrasound, milky white microbubbles suspended solution changed instantaneously to be clear. The interesting behavior of microbubbles observed in the ultrasonic field was investigated by microscopic and macroscopic visualizations. The rapid ascent of microbubbles was caused by their agglomeration, where the Bjerknes force of attraction and electrical repulsive force on microbubble surface acted. Ultrasonic irradiation into microbubble suspended solution was very useful for dynamic operation of microbubbles.