ナノ構造が制御された球状炭素微粒子の合成とエネルギー貯蔵デバイスへの応用

広島大学(Hiroshima University)博士(工学)Doctor of Engineeringdoctora

Videos on Carbon Particle Formation Prepared via Spray Pyrolysis

 These videos demonstrate the nanostructured carbon particle formation mechanism prepared through ultrasonic spray pyrolysis based on the self-assembly behavior of phenolic resin and polystyrene latex (PSL). By adjusting the attractive or repulsive forces between the phenolic resin and PSL particles, the morphology of the prepared carbon particles can be precisely controlled. Strong electrostatic attraction between the highly positively charged PSL and phenolic resin resulted in hollow carbon particles, while the electrostatic repulsion occurred in the presence of negatively charged PSL formed porous carbon particles. Depending on the requirements of different applications, using our strategy will in turn guide the synthesis of nanostructured carbon particles with desirable architectures and compositions.  </p

Enhanced Protein Adsorption Capacity of Macroporous Pectin Particles with High Specific Surface Area and an Interconnected Pore Network

There has been much interest in developing protein adsorbents using nanostructured particles, which can be engineered porous materials with fine control of the surface and pore structures. A significant challenge in designing porous adsorbents is the high percentage of available binding sites in the pores owing to their large surface areas and interconnected pore networks. In this study, continuing the idea of using porous materials derived from natural polymers toward the goal of sustainable development, porous pectin particles are reported. The template-assisted spray drying method using calcium carbonate (CaCO3) as a template for pore formation was applied to prepare porous pectin particles. The specific surface area was controlled from 177.0 to 222.3 m2 g-1 by adjusting the CaCO3 concentration. In addition, the effects of a macroporous structure, the specific surface area, and an interconnected pore network on the protein (lysozyme) adsorption capacity and adsorption mechanism were investigated. All porous pectin particles performed rapid adsorption (∼65% total capacity within 5 min) and high adsorption capacity, increasing from 1543 to the highest value of 2621 mg g-1. The results are attributed to the high percentage of available binding sites located in the macropores owing to their large surface areas and interconnected pore networks. The macroporous particles obtained in this study showed a higher adsorption capacity (2621 mg g-1) for lysozyme than other adsorbents. Moreover, the rapid uptake and high performance of this material show its potential as an advanced adsorbent for various macromolecules in the food and pharmaceutical fields

Multifunctional, Hybrid Materials Design via Spray-Drying : Much more than Just Drying

Spray-drying is a popular and well-known "drying tool" for engineers. This perspective highlights that, beyond this application, spray-drying is a very interesting and powerful tool for materials chemists to enable the design of multifunctional and hybrid materials. Upon spray-drying, the confined space of a liquid droplet is narrowed down, and its ingredients are forced together upon "falling dry." As detailed in this article, this enables the following material formation strategies either individually or even in combination: nanoparticles and/or molecules can be assembled; precipitation reactions as well as chemical syntheses can be performed; and templated materials can be designed. Beyond this, fragile moieties can be processed, or "precursor materials" be prepared. Post-treatment of spray-dried objects eventually enables the next level in the design of complex materials. Using spray-drying to design (particulate) materials comes with many advantages-but also with many challenges-all of which are outlined here. It is believed that multifunctional, hybrid materials, made via spray-drying, enable very unique property combinations that are particularly highly promising in myriad applications-of which catalysis, diagnostics, purification, storage, and information are highlighted

Multifunctional, Hybrid Materials Design via Spray‐Drying: Much more than Just Drying

Spray-drying is a popular and well-known “drying tool” for engineers. This perspective highlights that, beyond this application, spray-drying is a very interesting and powerful tool for materials chemists to enable the design of multifunctional and hybrid materials. Upon spray-drying, the confined space of a liquid droplet is narrowed down, and its ingredients are forced together upon “falling dry.” As detailed in this article, this enables the following material formation strategies either individually or even in combination: nanoparticles and/or molecules can be assembled; precipitation reactions as well as chemical syntheses can be performed; and templated materials can be designed. Beyond this, fragile moieties can be processed, or “precursor materials” be prepared. Post-treatment of spray-dried objects eventually enables the next level in the design of complex materials. Using spray-drying to design (particulate) materials comes with many advantages—but also with many challenges—all of which are outlined here. It is believed that multifunctional, hybrid materials, made via spray-drying, enable very unique property combinations that are particularly highly promising in myriad applications—of which catalysis, diagnostics, purification, storage, and information are highlighted

Synthesis of Submicron-Sized Spherical Silica-Coated Iron Nickel Particles with Adjustable Shell Thickness via Swirler Connector-Assisted Spray Pyrolysis

Silica-coated iron nickel (FeNi@SiO2) particles have attracted significant attention because of their potential applications in electronic devices. In this work, submicron-sized spherical FeNi@SiO2 particles with precisely controllable shell thickness were successfully synthesized for the first time using a swirler connector-assisted spray pyrolysis system, comprising a preheater, specific connector, and main heater. The results indicated that the thickness of the SiO2 shell can be tuned from 3 to 23 nm by adjusting the parameter conditions (i.e., preheater temperature, SiO2 supplied amount). Furthermore, our fabrication method consistently yielded a high coating ratio of more than 94%, indicating an excellent quality of the synthesized particles. Especially, to gain an in-depth understanding of the particle formation process of the FeNi@SiO2 particles, a plausible mechanism was also investigated. These findings highlight the importance of controlling the preheater and SiO2 supplied amount to obtain FeNi@SiO2 particles with desirable morphology and high coating quality

One-Step Aerosol Synthesis of SiO₂‑Coated FeNi Particles by Using Swirler Connector-Assisted Spray Pyrolysis

Silica-coated soft magnetic particles are essential for some powder magnetic cores consisting of primary (coarse particles) and secondary (fine particles) soft magnetic particles in the advancement of electric devices. Herein, we report the first investigation on the direct synthesis of submicron-sized silica-coated FeNi (FeNi@SiO2) particles as the secondary particle using a connector-assisted spray pyrolysis route. Provided by computational fluid dynamics calculation in applying different connector types, i.e., T-shaped and swirler, we found that the mixing performance between FeNi and HMDSO vapor in the swirler connector played an important role in resulting heterogeneous nucleation, which is crucial for obtaining the higher coating ratio (CR) and fewer undesired nanoparticles than that of the T-shaped connector. The as-prepared submicron-sized FeNi@SiO2 particles (353 nm) with the highest CR (95.9%) demonstrated a remarkable DC bias characteristic (Isat) and eddy current loss values on a powder magnetic core, promising the practical application in manufacturing soft magnetic components

Solid-state crystallization, oxygen-vacancy rich mesopores and stable triad-silanol nests in ZSM-5 catalyst induced by electron-beam irradiation and calcination

Mesopores and silanol nests are known two technological keys that essentially control the catalytic performance of ZSM-5 zeolite. However, designing and controlling them without using chemicals so that the produced ZSM-5 can have strongly enhanced catalytic properties and more importantly can be applied at industrial scale have still been a big challenge up to now. The present study employed the 10 MeV electron beam (EB) generated from an industrial linear accelerator to introduce both the O-vacancy rich mesopores and stable triad-silanol nests in ZSM-5. The structural modification of irradiated ZSM-5 samples was explored by using SEM and FTIR combined with positron annihilation spectroscopy (PAS) including positron annihilation lifetime (PAL), Doppler broadening (DB) of electron–positron annihilation energy and electron momentum distribution (EMD). Obtained results indicated that EB irradiation could recover the defective-crystal structure as well as intensively modify the structures of ZSM-5. In particular, the mechanism for the solid-state crystallization and the formation of the O-vacancy rich mesopores (maximum size of ∼4.5 nm) in ZSM-5 under the combined EB irradiation (10−110 kGy) and calcination (600 °C) was, for the first time, proposed. The mechanism for the formation of stable triad-silanol nests in the channels of irradiated and calcined ZSM-5 zeolites was also explored. The present study, therefore, opens a new research path of applying both EB irradiation and calcination to produce ZSM-5 with novel features for industrial catalytic application at large-production scale

Multimodal analysis of methylomics and fragmentomics in plasma cell-free DNA for multi-cancer early detection and localization

Despite their promise, circulating tumor DNA (ctDNA)-based assays for multi-cancer early detection face challenges in test performance, due mostly to the limited abundance of ctDNA and its inherent variability. To address these challenges, published assays to date demanded a very high-depth sequencing, resulting in an elevated price of test. Herein, we developed a multimodal assay called SPOT-MAS (screening for the presence of tumor by methylation and size) to simultaneously profile methylomics, fragmentomics, copy number, and end motifs in a single workflow using targeted and shallow genome-wide sequencing (~0.55×) of cell-free DNA. We applied SPOT-MAS to 738 non-metastatic patients with breast, colorectal, gastric, lung, and liver cancer, and 1550 healthy controls. We then employed machine learning to extract multiple cancer and tissue-specific signatures for detecting and locating cancer. SPOT-MAS successfully detected the five cancer types with a sensitivity of 72.4% at 97.0% specificity. The sensitivities for detecting early-stage cancers were 73.9% and 62.3% for stages I and II, respectively, increasing to 88.3% for non-metastatic stage IIIA. For tumor-of-origin, our assay achieved an accuracy of 0.7. Our study demonstrates comparable performance to other ctDNA-based assays while requiring significantly lower sequencing depth, making it economically feasible for population-wide screening