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We observed bilayer phase transitions of dimyristoylphosphatidylcholine (DMPC) in aqueous solutions of four kinds of monosaccharides, namely, D-glucose, D-fructose, D-allose and D-psicose, using differential scanning calorimetry (DSC). D-allose (C3-epimer of D-glucose) and D-psicose (C3-epimer of D-fructose) are rare sugars. We performed DSC measurements using two types of sugar-containing sample dispersions of the DMPC vesicles: one is a normal sample dispersion with no concentration asymmetry between the inside and outside of the vesicles and the other is an unusual sample dispersion with a concentration asymmetry. DSC measurements using normal sample dispersions with different sugar concentrations revealed that the temperatures and transition enthalpies of the pre- and main transition of the DMPC bilayer membrane did not significantly depend on the sugar concentration for all monosaccharides. DSC measurements using the unusual sample dispersions demonstrated that the concentration asymmetry caused the splitting of the endothermic peak of the main transition similarly irrespective of the sort of monosaccharides present. From all these DSC results, we conclude that (i) most monosaccharide molecules exist in the bulk water phase, (ii) no specific interaction depending on the molecular structure of each monosaccharide directly occurs between the DMPC and each monosaccharide molecule, and (iii) almost all the effects of the monosaccharides observed in this study are understandable as the general colligative properties of solutions.

Making ingestible devices edible facilitates diagnosis and therapy inside the body without the risk of retention; however, food materials are generally soft, absorb water molecules, and are not suitable for electronic devices. Here, we fabricated an edible water diffusion barrier film made by gelatin-beeswax composites for the encapsulation of transient electronics. Hydrophobic beeswax and hydrophilic gelatin are inherently difficult to mix; therefore, we created an emulsion simply by raising the temperature high enough to melt the materials and vigorous stirring them. As they cool, the beeswax with a relatively high solidification temperature aggregates and forms microspheres, which increases the gelatin gel's viscoelasticity and immobilizes the emulsion structure in the film. The thermoresponsive gelatin imparts degradability to the barrier and its stickiness also enables transfer of metal patterned electronics. Furthermore, we designed an edible resonator on the film and demonstrated its operation in an abdominal phantom environment; the resonator was made to be degradable in a warm aqueous solution by optimizing the composition ratio of the gelatin and beeswax. Our findings provide insight into criteria for making transient electronics on hydrophilic substrates with hydrophobic water diffusion barriers. This proof-of-concept study expands the potential of operating edible electronics in aqueous environments in harmony with the human body and nature.

The rare sugar D-allulose (Alu), with ca. 10% calories of sucrose (Suc), is a promising alternative sugar that can be used to improve the quality of starch gels in storage. The effects of Alu (compared to Suc) on the hardening and microstructural and molecular order of amylopectin-rich (glutinous rice (GR) and corn amylopectin (CAP)) and amylose-rich (corn (C)) starch gels were investigated. Alu and Suc both suppressed hardening in C gels, while Alu but not Suc was effective in GR and CAP gels. SEM results showed that Alu-containing GR and CAP maintained a relatively large pore size compared to Suc-containing gels. The deconvolution of FTIR spectra revealed that Alu-containing GR and CAP gels had lower ratios of intermolecular hydrogen bonds and higher ratios of loose hydrogen bonds than Suc-containing gels. For amylose-rich C gels, on the other hand, such tendencies were not observed. The influence of Alu on amylopectin-rich gels could be because Alu reduced the ratio of intermolecular hydrogen bonds, which might be involved in amylopectin recrystallization, and increased that of loose hydrogen bonds. The results suggest that Alu is more effective than Suc in inhibiting the hardening of amylopectin-rich starch gels during refrigerated storage.

In vitro reconstruction of highly mature engineered heart tissues (EHTs) is attempted for the selection of cardiotoxic drugs suitable for individual patients before administration. Mechanical contractile force generated in the EHTs is known to be a critical indicator for evaluating the EHT response. However, measuring contractile force requires anchoring the EHT in a tailored force-sensing cell culture chamber, causing technical difficulties in the stable evaluation of contractile force in long-term culture. This paper proposes a hydrogel-sheathed human induced pluripotent stem cell (hiPSC)-derived heart microtissue (H 3 M) that can provide an anchor-free contractile force measurement platform in commonly used multi-well plates. The contractile force associated with tissue formation and drug response is calculated by motion tracking and finite element analysis on the bending angle of the hydrogel sheath. From the experiment of the drug response, H 3 M is an excellent drug screening platform with high sensitivity and early testing capability compared to conventionally anchored EHT. This unique platform would be useful and versatile for regenerative therapy and drug discovery research in EHT., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)

The interstitial fluid of the skin contains glucose levels comparable to those of blood. Noninvasive glucose sensing by microwaves has great potential to relieve diabetics from the burden of daily blood sampling, but improving the selectivity of this method remains a challenge. This study reports a dielectrically equivalent multilayer skin phantom and provides insight into the criteria for noninvasive glucose sensing by conducting dielectric analysis. The skin phantom was a hydrogel composed of gelatin, glucose, sodium chloride, and water covered by paraffin-impregnated paper. Investigations conducted on a wide range of component concentrations revealed characteristic relative permittivity and dielectric loss determined by the amount of electrolyte and solution that was independent of the amount of glucose. Since the microwave response due to glucose tends to be buried in noise, we developed a flowchart that first identifies the amounts of electrolytes and proteins, which are the major components other than glucose, and then quantifies the remaining glucose content. This noninvasive glucose sensing method would not be limited to the medical healthcare field; it could potentially be used in food manufacturing processes, livestock farming, and plant cultivation management.

Ingestible electronics monitor biometric information from outside the body. Making them with harmless or digestible materials will contribute to further reducing the burden on the patient's oral intake. Here, considering that the inductive part plays an important role in communications, we demonstrate a degradable inductor fabricated with harmless substances. Such a transient component must meet conflicting requirements for both operation and disassembly. Therefore, we integrated a substrate made of gelatin, a thermally degradable material, and a precision coil pattern made of edible gold or silver leaf. However, gelatin itself lost its initial shape easily due to quick sol-gel changes in physiological conditions. Thus, we managed the gelatin's thermal responsiveness by using a tangle of gelatin/chitosan gel networks and genipin, an organic cross-linking agent, and gained insights into the criteria for developing transient devices with thermo-degradability. In addition, to compensate for the lack of water resistance and low conductivity of thin metal foils, we propose a laminated structure with oleogel (beeswax/olive oil). LCR resonance circuits, by connecting a commercial capacitor to the coil, worked wirelessly in the megahertz band and gradually degraded in a warm-water environment. The presented organic electronics will contribute to the future development of transient wireless communications for implantable and ingestible medical devices or environmental sensors with natural and harmless ingredients.

We developed a novel measuring and data-processing method for performing electrochemical surface plasmon resonance (EC-SPR) on sensor surfaces for which detecting a specific SPR angle is difficult, such as a polymer having a non-uniform thickness with coloration. SPR measurements are used in medicine and basic research as an analytical method capable of molecular detection without labeling. However, SPR is not good for detecting small molecules with small refractive index changes. The proposed EC-SPR, which combines SPR measurements with an electrochemical reaction, makes it possible to measure small molecules without increasing the number of measurement steps. A drawback of EC-SPR is that it is difficult to detect a specific SPR angle on electron mediators, and it was found that it may not be possible to capture all the features produced. The novel method we describe here is different from the conventional one in which a specific SPR angle is obtained from an SPR curve; rather, it processes the SPR curve itself and can efficiently aggregate the feature displacements in the SPR curves that are dispersed through multiple angles. As an application, we used our method to detect small concentrations of H 2 O 2 (LOD 0.7 μM) and glutamate (LOD 5 μM).

A critical microchannel technique is to isolate specific objects, such as cells, in a biological solution. Generally, this particle sorting is achieved by designing a microfluidic device and tuning its control values; however, unpredictable motions of the particle mixture make this approach time-consuming and labor intensive. Here, we show that microfluidic control with reinforced learning characterized by utilizing failure results can maximize the training effect with limited data. This method uses microscopic images of the separation process, including failed conditions (inappropriate flow speeds or dilution rates of biological samples), and insights for efficient learning are provided by setting gradient rewards according to the degree of failure. Once learning is performed in this manner, the optimal separating condition for other related samples can be automatically found. Failed experiments are not wasteful; they increase training data and make it easier to reach correct answers. This device control could be useful in automatic synthetic chemistry, biomedical analysis, and microfabrication robotics.

This paper describes up-scalable microfiber-shaped tissues for macroscale tendon tissue reconstruction in vitro. C3H10T1/2 cells were encapsulated in a calcium alginate hydrogel microfiber that was fabricated via a double coaxial microfluidic device. The C3H10T1/2 cells gradually merged to construct the microfiber-shaped tendon-like tissue. Our microfiber-shaped tendon-like tissues were alive and maintained their microfiber-shaped morphology over 600 days. Immunostaining and real-time quantitative polymerase chain reaction analyses showed that our fabricated microfiber-shaped tendon-like tissue properly expressed tenomodulin and the orientation of the filaments of actin, which are one of the characteristics of tendon tissue in vivo. Furthermore, a macroscale tendon tissue assembly with ∼1 cm in length and ∼200 µm in thickness was successfully constructed by bundling the microfiber-shaped tendon-like tissues together. This feature enabled us to fabricate a macroscale tendon tissue with uniform cell distribution. We believe that our fabricated microfiber-shaped tendon-like tissue would be a suitable strategy to reconstruct tendon tissue in vitro for the treatments of tendon-related injuries., (© 2022 Wiley Periodicals LLC.)

Scientists who design chemical substances often use materials informatics (MI), a data-driven approach with either computer simulation or artificial intelligence (AI). MI is a valuable technique, but applying it to layered structures is difficult. Most of the proposed computer-aided material search techniques use atomic or molecular simulations, which are limited to small areas. Some AI approaches have planned layered structures, but they require a physical theory or abundant experimental results. There is no universal design tool for multilayer films in MI. Here, we show a multilayer film can be designed through machine learning (ML) of experimental procedures extracted from chemical-coating articles. We converted material names according to International Union of Pure and Applied Chemistry rules and stored them in databases for each fabrication step without any physicochemical theory. Compared with experimental results which depend on authors, experimental protocol is superiority at almost unified and less data loss. Connecting scientific knowledge through ML enables us to predict untrained film structures. This suggests that AI imitates research activity, which is normally inspired by other scientific achievements and can thus be used as a general design technique., (© 2022. The Author(s).)