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1.
J Am Chem Soc ; 2024 Jun 27.
Article in English | MEDLINE | ID: mdl-38934730

ABSTRACT

With the growing demand for postsilicon electronics, the purification of single-walled carbon nanotubes (SWCNTs) in terms of their chirality, which defines their atomic and electronic structure, is becoming increasingly important. Herein, we demonstrate the selective extraction of high-quality semiconducting SWCNTs using alkyl cellulose as a dispersant in organic solvents. We investigated the separation factors of dispersant structures, such as the degree of substitution (DS) and molecular weight, and clarified the appropriate dispersant structures, such as moderately substituted hexyl cellulose, for selective semiconducting SWCNT extraction. Due to the improved purity and quality of the semiconducting SWCNTs obtained by this method, their films exhibit excellent thermoelectric power factors, outperforming not only unsorted SWCNTs but also conducting polymer-sorted SWCNTs. This sorting technology paves the way for supplying high-quality semiconducting SWCNTs in a viable manner.

3.
J Phys Chem Lett ; 13(7): 1879-1885, 2022 Feb 24.
Article in English | MEDLINE | ID: mdl-35175057

ABSTRACT

Metallic iron (Fe) represents an exceptionally active catalyst, as shown in its use in the Haber-Bosch process to dissociate nitrogen molecules; however, the ease of corrosion by oxidation limits its usage. Hence, in most applications using metallic Fe catalysts, hydrogen is a necessary reactant. We report a novel hydrogen-free approach to fabricating reduced, highly active, and corrosion-resistive Fe-based catalysts using trace levels of noble metals (NMs) such as Ir, Rh, and Pt confined in the nanoparticle (NP). X-ray photoelectron spectroscopy (XPS) revealed that as little as ∼0.3 atom % was sufficient to induce the reduction of Fe. Extensive XPS analysis showed that the reduced NM atoms segregated to the NP surface and reduced the surrounding Fe atoms. We demonstrated the catalytic activity of the nanoparticles by the efficient synthesis of submillimeter tall, vertically aligned, and mainly double-walled carbon nanotube arrays using a completely hydrogen-free chemical vapor deposition process.

4.
Org Biomol Chem ; 20(10): 2043-2047, 2022 03 09.
Article in English | MEDLINE | ID: mdl-35005766

ABSTRACT

The effects of a crowded environment on DNA-mediated electron transfer were evaluated using a pyrene-modified oligonucleotide containing a hole-trapping nucleobase in poly(ethylene glycol) mixed solutions. Rapid decompositions of hole-trapping bases in condensed and noncondensed DNA showed that more efficient electron transfer occurred under crowded conditions than in dilute solutions.


Subject(s)
DNA
5.
Nanomaterials (Basel) ; 11(12)2021 Dec 20.
Article in English | MEDLINE | ID: mdl-34947810

ABSTRACT

We present a study quantitatively demonstrating that the method of synthesis (gas phase, fixed bed, non-fixed bed) represents a determining factor in the level of crystallinity in growing single wall carbon nanotubes (SWCNTs). Using far infrared spectroscopy, the "effective length" (associated with the level of crystallinity) was estimated for CNTs grown using various synthetic methods (lab-produced and supplemented by commercially purchased SWCNTs) as a metric for crystallinity (i.e., defect density). Analysis of the observed "effective lengths" showed that the SWCNTs fell into two general groups: long and short (high and low crystallinity) synthesized by gas-phase methods and all other supported catalyst methods, respectively. Importantly, the "long" group exhibited effective lengths in the range of 700-2200 nm, which was greater than double that of the typical values representing the "short" group (110-490 nm). These results highlight the significant difference in crystallinity. We interpret that the difference in the crystallinity stemmed from stress concentration at the nanotube-catalyst interface during the growth process, which originated from various sources of mismatch in growth rates (e.g., vertically aligned array) as well as impact stress from contact with other substrates during fluidization or rotation. These results are consistent with well-accepted belief, but now are demonstrated quantitatively.

6.
ACS Omega ; 6(29): 18763-18769, 2021 Jul 27.
Article in English | MEDLINE | ID: mdl-34337216

ABSTRACT

The importance of hydrogen in carbon nanotube (CNT) synthesis has been known as it supports the critical processes necessary for CNT growth, such as catalyst reduction. However, within the scope of our mini microplasma CNT synthesis reactor, we found that hydrogen was critical for unexpected reasons. Without hydrogen, CNT growth was inhibited and characterized by amorphous carbon particles. Optical emission spectroscopy of the microplasma revealed that without hydrogen, the high-energy electrons induced the immediate decomposition of carbon feedstock simultaneously with the catalyst feedstock, thus suppressing the formation of catalyst nanoparticles and inducing catalyst deactivation. In contrast, the inclusion of hydrogen induced less-immediate decomposition of reactant gases, through the conversion of electron energy of the plasma to thermal energy, which provided the appropriate conditions for catalyst nanoparticle formation and subsequent CNT nucleation. A simple reaction pathway model was proposed to explain these observed results and underlying mechanisms.

7.
Clin Exp Nephrol ; 25(9): 1027-1034, 2021 Sep.
Article in English | MEDLINE | ID: mdl-34061287

ABSTRACT

BACKGROUND: Serum adiponectin circulates in three multimeric isoforms: high-molecular-weight (HMW), middle-molecular-weight (MMW), and low-molecular-weight (LMW) isoforms. Potential change in the circulating adiponectin levels in patients with nephrotic syndrome (NS) remain unknown. This study aimed to assess the levels of total adiponectin and the distribution of its isoforms in pediatric patients with NS. METHODS: We sequentially measured total adiponectin and each adiponectin isoform levels at the onset of NS, initial remission, and during the remission period of the disease in 31 NS patients. We also calculated the ratios of HMW (%HMW), MMW (%MMW), and LMW (%LMW) to total adiponectin incuding 51 control subjects. RESULTS: The median of total serum adiponectin levels in patients were 36.7, 36.7, and 20.2 µg/mL at the onset, at initial remission, and during the remission period of NS, respectively. These values were significantly higher than those in control subjects. The median values of %HMW, %MMW, and %LMW values were 56.9/27.0/14.1 at the onset, 62.0/21.8/13.4 at the initial remission, and 58.1/21.7/17.5 at during the remission period of NS, respectively. Compared with control subjects, %HMW at initial remission and %MMW at the onset were high, and the %LMW values at the onset and at initial remission were low. CONCLUSIONS: In patients with NS, total serum adiponectin levels increase at the onset of the disease, and the ratio of adiponectin isoforms changes during the course of the disease. Further studies are needed to delineate the mechanisms between proteinuria and adiponectin isoforms change.


Subject(s)
Adiponectin/blood , Nephrotic Syndrome/blood , Nephrotic Syndrome/drug therapy , Anti-Inflammatory Agents/therapeutic use , Case-Control Studies , Child , Child, Preschool , Female , Humans , Infant , Male , Molecular Weight , Prednisolone/therapeutic use , Protein Isoforms/blood , Remission Induction
8.
Pharmaceutics ; 13(2)2021 Jan 27.
Article in English | MEDLINE | ID: mdl-33513827

ABSTRACT

The polymer that includes 2-methacryloyloxy ethyl phosphorylcholine (MPC) is well-known as an effectively hydrating multifunction agent. In this study, we prepared an MPC polymer (MPCP) using radical polymerization with co-monomers-MPC/Stearyl Methacrylate/N,N-dimethylacrylamide-and evaluated the MPCP's usefulness for dry eye treatment using a rabbit model treated with N-acetylcysteine. The MPCP particle size was 50-250 nm, and the form was similar to that of micelles. The MPCP viscosity (approximately 0.95 mPa·s) was 1.17-fold that of purified water, and a decrease in the transepithelial electrical resistance value (corneal damage) was not observed in the immortalized human corneal epithelial cell line HCE-T cell (HCE-T cell layer). The MPCP enhanced the water maintenance on the cornea, and the instillation of MPCP increased the lacrimal fluid volume and prolonged the tear film breakup time without an increase in total mucin contents in the lacrimal fluid of the normal rabbits. The therapeutic potential of the MPCP for dry eye was evaluated using an N-acetylcysteine-treated rabbit model, and, in our investigation, we found that MPCP enhanced the volume of lacrimal fluid and promoted an improvement in the tear film breakup levels. These findings regarding the creation and characteristics of a novel MPCP will provide relevant information for designing further studies to develop a treatment for dry eyes.

9.
SAGE Open Med Case Rep ; 8: 2050313X20969559, 2020.
Article in English | MEDLINE | ID: mdl-33294189

ABSTRACT

Hyponatremic hypertensive syndrome is characterized by hypertension, hyponatremia, and hypokalemia due to unilateral renal artery stenosis. We herein report a 1-year-old hyponatremic hypertensive syndrome infant without persistent hypertension in the acute phase. On the ninth hospital day, his systolic and diastolic blood pressure increased up to 154-160 and 70-84 mmHg, respectively. Acute gastroenteritis and dehydration might transiently mask his hypertension. By percutaneous transluminal balloon angioplasty for right renal artery, his blood pressure finally normalized without antihypertensive drugs. We reviewed 23 previously reported pediatric patients with hyponatremic hypertensive syndrome under the age of 15 years. Including our patient, there are only three reports on hyponatremic hypertensive syndrome without persistent hypertension in the acute phase. Hyponatremic hypertensive syndrome is curable with proper diagnosis and timely intervention. Therefore, pediatricians should pay attention to the signs and symptoms associated with hyponatremic hypertensive syndrome, even if persistent hypertension was absent in the acute phase.

10.
Org Biomol Chem ; 18(36): 7183-7187, 2020 09 23.
Article in English | MEDLINE | ID: mdl-32897281

ABSTRACT

It is known that double-stranded DNA (dsDNA) turns into a liquid crystalline phase by the addition of a high concentration of polymer with salt. SYBR Green I (SG) is a well-known sensitive fluorescent stain for dsDNA, and is intercalated in liquid crystalline DNA. Formation of the liquid crystalline dsDNA-SG complex has been confirmed by CD spectral measurements, fluorescence spectral measurements and confocal fluorescence microscopy. SG in dsDNA was also used as a singlet oxygen generator. We conducted photoirradiation experiments using three kinds of 42-mer oligonucleotides with SG. The amount of guanine decomposition by selective irradiation of SG was analyzed using HPLC after digestion of dsDNA in each sample solution. We found that singlet oxygen produced in liquid crystalline DNA promoted guanine damage much more efficiently than in homogeneous solution.


Subject(s)
Singlet Oxygen
11.
Heliyon ; 6(6): e04211, 2020 Jun.
Article in English | MEDLINE | ID: mdl-32577575

ABSTRACT

OBJECTIVES: The effects of 2-methacryloyloxyethyl phosphorylcholine (MPC)-polymer on the adherence of microorganisms such as non-Candida albicans Candida (NCAC) and methicillin-resistant Staphylococcus aureus (MRSA), frequently detected in oral infections in immunocompromised and/or elderly people, to denture resin material, are still unclear. Here, we report the effects of MPC-polymer on the adherence of C. albicans, NCAC, and MRSA to acrylic denture resin. METHODS: Sixteen strains of C. albicans, seven strains of C. glabrata, two strains of C. tropicalis, one strain of C. parapsilosis, and six strains of MRSA were used. We cultured the fungal/bacterial strains and examined the cell growth and adherence of fungi/bacteria to mucin-coated acrylic denture resin plates (ADRP) with or without MPC-polymer coating, by scanning electron microscopy. The cell surface hydrophobicity of the fungal/bacterial strains was measured by the adsorption to hydrocarbons. RESULTS: MPC-polymer did not affect the growth of all strains of Candida species and MRSA, but significantly suppressed adherence to ADRP in most strains of C. albicans and all strains of NCAC and MRSA. A significant positive correlation was found between cell hydrophobicity and the reduction rates of microbial adherence to ADRP treated with 5% of MPC-polymer. CONCLUSIONS: MPC-polymer treatment for acrylic resin material suppresses the adherence of C. albicans, NCAC and MRSA via their hydrophilicity interaction. CLINICAL SIGNIFICANCE: The application of MPC-polymer for denture hygiene is potent to prevent oral candidiasis, denture stomatitis and opportunistic infection, caused by Candida species and MRSA, via suppressing the adherence of those fungus/bacteria.

12.
Org Biomol Chem ; 18(1): 47-51, 2019 12 18.
Article in English | MEDLINE | ID: mdl-31799580

ABSTRACT

Spermidine, a trivalent organic cation, induced DNA structural changes and suppressed guanine photooxidative decomposition via electron transfer through pyrene-modified DNA. On the other hand, adding higher concentrations of spermidine resulted in DNA condensation. The efficiency of guanine decomposition in condensed pyrene-modified DNA was promoted remarkably.


Subject(s)
DNA/chemistry , Guanine/chemistry , Spermidine/chemistry , Electron Transport , Photochemical Processes
13.
Chem Commun (Camb) ; 55(53): 7695-7698, 2019 Jul 07.
Article in English | MEDLINE | ID: mdl-31204743

ABSTRACT

We investigated the effects of a crowded environment on guanine oxidation in pyrene-modified oligonucleotides by photoinduced electron transfer. We observed drastic promotion of guanine oxidation in Ψ (psi; polymer- and salt-induced)-type DNA.


Subject(s)
DNA/chemistry , Guanine/chemistry , Electron Transport , Oxidation-Reduction
14.
Nanoscale Adv ; 1(10): 4076-4081, 2019 Oct 09.
Article in English | MEDLINE | ID: mdl-36132090

ABSTRACT

Here, we demonstrate an approach of increasing the density of ultralong carbon nanotube (CNT) growth by combining a fast-heating method developed by Huang et al. (J. Am. Chem. Soc., 2003, 125, 5636-5637) with catalyst support engineering. Specifically, using graphene oxide as a catalyst support for iron oxide (Fe3O4) catalyst nanoparticles, we achieved high density growth of CNTs grown by the "kite-mechanism". Our analysis revealed that the fast-heating method reduced undesired aggregation of the catalyst nanoparticles, which has been reported to be a primary limitation mechanism, by shortening the time between substrate heating and CNT growth. In addition, the use of the graphene oxide support led to controllable and uniform dispersion of catalyst nanoparticles in relatively high density which provided increased process control by extending the time before the onset of catalyst aggregation. Together, these approaches suppressed the aggregation of the catalyst nanoparticles, which facilitated the "tip-growth" mode instead of the "root-growth" mode, and led to the high density growth of ultralong CNTs. Our results also indicate additional limitations and complexities on the high density CNT growth by the kite-growth approach, which limit high density synthesis.

15.
J Am Chem Soc ; 140(3): 1098-1104, 2018 01 24.
Article in English | MEDLINE | ID: mdl-29272113

ABSTRACT

We report a general strategy to fabricate highly concentrated, viscoplastic and stable suspensions by designing the particle surface structure to control the interparticle attractive forces. Unlike conventional methods, where the choice of solvent is critical in balancing interparticle interactions, suspensions showing excellent stability and viscoplastic properties were made using various solvents. We demonstrated this approach using highly sparse agglomerates of carbon nanotubes (CNTs) as the particles. Our results revealed that the essential feature of the CNT agglomerate to fabricate these suspensions was high porosity with a spacing size much smaller than the overall size, which was only possible using long single-walled carbon nanotubes (SWNTs). In this way, the agglomerate surface was characterized by fine network of CNT bundles. These suspensions exhibited solid-like behavior at rest (characterized by a high yield stress of c.a. 100 Pa) and a liquid-like behavior when subjected to a stress (characterized by a significant drop of an apparent viscosity to 1 Pa·s at a shear rate of 1000 s-1). Furthermore, in contrast to conventionally fabricated suspensions, these "CNT pastes" exhibited exceptional stability at rest, under flow, and at extremely high concentrations during the drying process, with only a weakly observable dependence on solvent type. As a result, highly uniform micrometer-thick SWNT films were successfully fabricated by dried blade-coated films of these pastes. Finally, we developed a simple, semiempirical model and clarified the importance of the CNT agglomerate microstructure (the ratio of spacing size/particle size and porosity) on tailoring the cohesive forces between particles to fabricate stable viscoplastic suspensions.

16.
Nanoscale ; 9(44): 17617-17622, 2017 Nov 16.
Article in English | MEDLINE | ID: mdl-29115340

ABSTRACT

Recently, the millimetre-scale, highly efficient synthesis of single-wall carbon nanotube (SWCNT) forests from Fe catalysts has been reported through the annealing of the magnesia (MgO) underlayer. Here, we report the double-edged effects of underlayer annealing on the efficiency and structure of the SWCNT forest synthesis through a temperature-dependent examination. Our results showed that the efficiency of the SWCNT forests sharply increased with increased underlayer annealing temperatures from 600 °C up to 900 °C due to a temperature-dependent structural modification, characterized by increased grain size and reduced defects, of the MgO underlayer. Beyond this temperature, the SWCNT fraction also decreased as a result of further structural modification of the MgO underlayer. This exemplifies the double-edged effects of annealing. Specifically, for underlayer annealing below 600 °C, the catalyst subsurface diffusion was found to limit the growth efficiency, and for excessively high underlayer annealing temperatures (>900 °C), catalyst coalescence/ripening led to the formation of double-wall carbon nanotubes. As a result, three distinct regions of synthesis were observed: (i) a "low yield" region below a threshold temperature (∼600 °C); (ii) an "increased yield" region from 600 to 900 °C, and (iii) a "saturation" region above 900 °C. The efficient SWCNT forest synthesis could only occur within a specific annealing temperature window as a result of this double-edged effects of underlayer annealing.

17.
J Infect Chemother ; 23(8): 517-522, 2017 Aug.
Article in English | MEDLINE | ID: mdl-28528936

ABSTRACT

Although carbapenem is the recommended for urinary tract infection (UTI) caused by extended-spectrum beta-lactamase (ESBL)-producing organisms, non-carbapenems have been reported to be effective for adult patients with UTI caused by ESBL-producing organisms. The purpose of this study was to evaluate the efficacy of non-carbapenems for pediatric patients with UTI due to ESBL-producing Escherichia coli (E. coli) based on the microbiologic and clinical outcomes. Fifteen children, who were treated for first febrile UTI caused by ESBL-producing E. coli were enrolled in this study. Antimicrobial susceptibilities and ESBL production were determined according to the Clinical and Laboratory Standards Institute guidelines. To detect CTX-M genes, polymerase chain reaction was performed with specific primers for blaCTX-M detection. Of the 15 enrolled patients, 10 (66.7%) were boys and 5 (33.3%) were girls, with a median age of four months. VUR was detected in six patients (40%). For detection of blaCTX-M by PCR, CTX-M-3, CTX-M-8, CTX-M-14, and CTX-M-15 were detected in five, one, eight, and one patient, respectively. Overall, 14 of the 15 isolates (93.3%) were susceptible for fosfomycin (FOM), and all isolates were susceptible for cefmetazole (CMZ), flomoxef (FMOX), and imipenem/cilastatin (IPM/CS). Of the 15 patients, 12 (80%) clinically improved without the use of carbapenems. In conclusion, even if isolates of ESBL-producing E. coli are multidrug resistant based on MIC assessment, clinical susceptibility to non-carbapenems, such as CMZ, FMOX, and FOM, is possible. Accordingly, carbapenems may not be required all the time for treatment of pediatric UTI in clinical practice.


Subject(s)
Anti-Bacterial Agents/therapeutic use , Carbapenems/therapeutic use , Escherichia coli Infections/drug therapy , Escherichia coli , Urinary Tract Infections/drug therapy , Child, Preschool , Escherichia coli Infections/microbiology , Female , Fever , Humans , Infant , Japan/epidemiology , Male , Retrospective Studies , Urinary Tract Infections/microbiology , beta-Lactamases
19.
Clin Exp Nephrol ; 21(4): 671-676, 2017 Aug.
Article in English | MEDLINE | ID: mdl-27558467

ABSTRACT

BACKGROUND: In patients with complicated steroid-dependent nephrotic syndrome (SDNS), rituximab (RTX) followed by immunosuppressive agent (IS) can maintain remission without the use of prednisolone (PSL). However, available data on the predictive factors for relapse and the long-term outcome after this protocol are few. METHODS: We retrospectively analyzed 43 SDNS patients who were followed-up for a long time (>2 years, mean 5.4 years) after a single dose of RTX (375 mg/m2) from September 2007. After RTX, PSL was tapered off within 6 months; monotherapy with IS, such as cyclosporine or mycophenolate mofetil, was continued to prevent post-RTX relapse. For patients who achieved >12 months of PSL-free remission, IS was also tapered off. RESULTS: Thirty-nine patients (91 %) could discontinue PSL without relapses at a median of 154 days after the initial RTX. The first relapse of NS occurred in 39 patients (91 %) at a median of 586 days; additional RTX doses were administered in 28 patients (65 %). Kaplan-Meier analysis showed that shorter CD19 cell depletion (<150 days) and younger age at RTX initiation (<12.5 years) were significantly associated with high risk for first relapse after RTX (log rank p < 0.05). In multivariate analysis, mycophenolate mofetil therapy as maintenance IS after RTX was the only predicted risk factor for first relapse (hazard ratio 2.75; p = 0.027). At the last follow-up, IS was still used in 33 patients (77 %); treatment-free remission (>12 months) was achieved in only five patients (12 %). CONCLUSIONS: The introduction of RTX may not be necessarily associated with improved long-term outcome.


Subject(s)
Glucocorticoids/administration & dosage , Immunologic Factors/administration & dosage , Nephrotic Syndrome/drug therapy , Prednisolone/administration & dosage , Rituximab/administration & dosage , Adolescent , Age Factors , Child , Child, Preschool , Cyclosporine/administration & dosage , Disease-Free Survival , Drug Administration Schedule , Drug Therapy, Combination , Female , Glucocorticoids/adverse effects , Humans , Immunologic Factors/adverse effects , Immunosuppressive Agents/administration & dosage , Japan , Kaplan-Meier Estimate , Male , Nephrotic Syndrome/diagnosis , Nephrotic Syndrome/immunology , Prednisolone/adverse effects , Proportional Hazards Models , Recurrence , Retrospective Studies , Risk Factors , Rituximab/adverse effects , Time Factors , Treatment Outcome
20.
J Am Chem Soc ; 138(51): 16608-16611, 2016 12 28.
Article in English | MEDLINE | ID: mdl-27977184

ABSTRACT

An unexpected 5000% increase in growth efficiency and high (95%) single-wall selectivity synthesis of vertically aligned carbon nanotubes (CNTs) was shown from Fe catalysts supported on a sputtered MgO underlayer from a simple underlayer treatment, i.e., annealing treatment. In this way, millimeter-scale single-wall carbon nanotube "forests" could be synthesized in a 10 min time, which has never been previously reported for MgO catalyst underlayer or any underlayer besides Al2O3. This level of efficiency and characterized SWCNT properties were similar to those grown using Al2O3 underlayers. Spectroscopic and microscopic analyses revealed that the treatment improved stability of the catalyst nanoparticle array by the suppressing catalyst subsurface diffusion and retaining the metallic state of the surface Fe atoms. Taken together, these results reveal a new route in achieving highly efficient SWCNT synthesis.

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