Publications by authors named "Takanori Suzuki"

109 Publications

Sodium-containing versus sodium-trace preparations of IVIG for children with Kawasaki disease in the acute phase.

Eur J Pediatr 2021 May 10. Epub 2021 May 10.

Department of Clinical Epidemiology and Health Economics, School of Public Health, The University of Tokyo, Tokyo, Japan.

Kawasaki disease (KD) is an acute systemic vasculitis that most commonly causes acquired cardiac disease in children in developed countries. The most highly recommended treatment for KD is 2 g/kg intravenous immunoglobulin (IVIG). There are two types of IVIG, sodium-containing (high-Na) and sodium-trace (low-Na) preparations. However, few studies have compared the effects of these two preparations for superiority. The purpose of this study was to compare outcomes between high and low-Na IVIG preparations in KD children using a national inpatient database in Japan. We used the Diagnostic Procedure Combination database to identify KD patients treated with IVIG between 2010 and 2017. We identified those receiving high and low-Na preparations of IVIG as an initial treatment. Outcomes included proportion of coronary artery abnormalities (CAA), IVIG resistance, adverse effects, length of stay, and medical cost. Propensity score-matched analyses were conducted to compare the outcomes between the two groups. Instrumental variable analyses were performed to confirm the results. We identified 42,345 patients with KD. There were significant differences in proportions of CAA (2.8% vs. 3.2%; p = 0.031) and IVIG resistance (17% vs. 18%, p = 0.001) between the two groups. However, there were no significant differences in length of stay or medical cost. The instrumental variable analysis confirmed the same results as the propensity score analysis.Conclusion: The present study suggests that high-Na IVIG is potentially effective for reducing the proportion of CAA in KD patients. Prospective studies are warranted to confirm the effectiveness observed in this study. What is Known: • For treatments of Kawasaki Disease in acute phase, intravenous immunoglobulin have been the most recommended to reduce fever early and prevent complications of coronary artery abnormalities. There are two types of IVIG preparations, sodium-containing IVIG and sodium-trace IVIG. However, few studies have performed comparisons to determine which preparation of IVIG is superior. What is New: • The present findings suggest that high-Na IVIG is associated with reductions in the proportions of CAAs and IVIG resistance in KD patients.
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http://dx.doi.org/10.1007/s00431-021-04096-xDOI Listing
May 2021

Clinical efficacy of a novel, high-sensitivity HBcrAg assay in the management of chronic hepatitis B and HBV reactivation.

J Hepatol 2021 Mar 21. Epub 2021 Mar 21.

Department of Clinical Laboratory Medicine, Nagoya City University Hospital, Nagoya, Japan; Department of Virology and Liver Unit, Nagoya City University Graduate School of Medical Sciences, Nagoya, Japan; Department of Gastroenterology and Hepatology, Faculty of Life Sciences, Kumamoto University, Kumamoto, Japan. Electronic address:

Background & Aims: A fully automated, novel high-sensitivity hepatitis B core-related antigen assay (iTACT-HBcrAg) has been developed. We demonstrate the clinical utility of iTACT-HBcrAg for monitoring chronic hepatitis B (CHB) and for the early detection of HBV reactivation.

Methods: After fundamental assessments, the clinical performance of iTACT-HBcrAg was compared with other HBV markers. i) Serial sera, available from 161 HBeAg-negative patients with CHB and persistently undetectable HBV DNA, were measured by iTACT-HBcrAg and a conventional HBcrAg assay (G-HBcrAg). ii) Serial sera from 13 HBV-reactivated patients were measured by iTACT-HBcrAg and an ultra-high-sensitivity HBsAg immune complex transfer-chemiluminescent enzyme immunoassay (lower limit of detection; 0.0005 IU/ml, ICT-CLEIA) to compare HBV DNA detection. iii) To elucidate the various HBcrAg components detected by iTACT-HBcrAg, OptiPrep density gradient centrifugation analysis was performed on sera obtained before and after HBV reactivation.

Results: The analytical performance of iTACT-HBcrAg was satisfactory. The sensitivity of iTACT-HBcrAg (2.1 Log U/ml) was approximately 10-fold greater than that of G-HBcrAg (2.8 Log U/ml). i) HBcrAg was detectable in the sera of 97.5% (157/161) of patients with CHB by iTACT-HBcrAg, of whom 75.2% (121/161) had ≥2.8 Log U/ml HBcrAg and 22.4% (36/161) had 2.1-2.8 Log U/ml HBcrAg, which was undetectable by G-HBcrAg. ii) 9 and 2 of 13 HBV-reactivated patients were HBcrAg-positive by iTACT-HBcrAg before and at HBV DNA positivity, respectively; 7 and 4 were HBcrAg-positive by iTACT-HBcrAg before and at HBsAg-positivity by ICT-CLEIA, respectively. iii) The HBcrAg detected by iTACT-HBcrAg before HBV reactivation was contained in empty particles (22 KDa precore protein).

Conclusions: iTACT-HBcrAg could be used to better monitor responses to anti-HBV treatments in HBeAg-negative patients and for the early detection of HBV reactivation.

Lay Summary: A fully automated, novel high-sensitivity hepatitis B core-related antigen assay (iTACT-HBcrAg) has been developed. iTACT-HBcrAg can be used to monitor HBeAg-negative patients with chronic hepatitis B, as well as for the early detection of HBV reactivation. iTACT-HBcrAg could be used as a general marker of disease progression and treatment response.
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http://dx.doi.org/10.1016/j.jhep.2021.02.017DOI Listing
March 2021

Hysteretic Three-State Redox Interconversion among Zigzag Bisquinodimethanes with Non-fused Benzene Rings and Twisted Tetra-/Dications with [5]/[3]Acenes Exhibiting Near-Infrared Absorptions.

J Am Chem Soc 2021 Mar 26;143(9):3306-3311. Epub 2021 Feb 26.

Department of Chemistry, Faculty of Science, Hokkaido University, Sapporo 060-0810, Japan.

Octaaryl-substituted bisquinodimethanes (BQDs) with a zigzag structure were designed as redox-switchable molecules that undergo four-electron oxidation to produce tetracationic pentacenes with a doubly twisted structure. In contrast to one-stage four-electron oxidation of BQDs, stepwise two-electron reduction of tetracationic pentacenes occurs to give dicationic anthracenes and then the original BQDs, step-by-step. Since both tetracations and dications exhibit near-infrared (NIR) absorptions (-1400 nm) based on an intramolecular charge-transfer interaction, changes in not only their structures but also their UV-vis-NIR spectra can be controlled by redox stimuli. In this Communication, we present an unprecedented one-step π-extension to pentacene from non-fused benzene rings by oxidation, and subsequent two-stage deannulation to benzene rings via anthracene upon reduction. All structures were determined by single-crystal X-ray analyses, and their properties were characterized by spectroscopic and theoretical studies.
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http://dx.doi.org/10.1021/jacs.1c00189DOI Listing
March 2021

Heterocyclic Ring-Opening of Nanographene on Au(111).

Angew Chem Int Ed Engl 2021 Apr 12;60(17):9427-9432. Epub 2021 Mar 12.

Research Center for Advanced Measurement and Characterization, National Institute for Materials Science, 1-2-1 Sengen, Tsukuba, Ibaraki, 305-0047, Japan.

Cyclo-dehydrogenation is of importance to induce the planarization of molecules on noble surfaces upon annealing. In contrast to a number of successful syntheses of polycyclic aromatic hydrocarbons by forming carbon-carbon bonds, it is still rare to conduct conjugation and cleavage of carbon-nitrogen bonds in molecules. Here, we present a systematic transformation of the C-N bonds in11,11,12,12-tetraphenyl-1,4,5,8-tetraazaanthraquinodimethane as well as three other derivatives on Au(111). With bond-resolved scanning tunneling microscopy, we discovered novel the "heterocyclic segregation" reaction of one pyrazine ring with two nitrogen atoms to form two quinoline rings with one nitrogen each. Density functional theory calculations showed that the intramolecular ring-forming and -opening of N-heterocycles are strongly affected by the initial hydrogen-substrate interaction.
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http://dx.doi.org/10.1002/anie.202017137DOI Listing
April 2021

Identification of synthetic inhibitors for the DNA binding of intrinsically disordered circadian clock transcription factors.

Chem Commun (Camb) 2020 Sep;56(76):11203-11206

Academic Assembly, Institute of Agriculture, Shinshu University, 8304 Minami-Minowa, Kami-Ina, Nagano 399-4598, Japan.

Essential components of the human circadian clock, BMAL1 and CLOCK, which are intrinsically disordered transcription factors, were expressed and subjected to a fluorescent in vitro binding assay using an E-box DNA fragment. Screening of a chemical library identified 5,8-quinoxalinedione (1), which was found to inhibit binding of the heterodimer BMAL1/CLOCK to E-box at low micromolar concentrations.
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http://dx.doi.org/10.1039/d0cc04861eDOI Listing
September 2020

High-dose versus low-dose intravenous immunoglobulin for treatment of children with Kawasaki disease weighing 25 kg or more.

Eur J Pediatr 2020 Dec 29;179(12):1901-1907. Epub 2020 Aug 29.

Department of Health Policy and Informatics, Graduate School of Medicine, Tokyo Medical and Dental University, Tokyo, Japan.

Little is known whether 2-g/kg IVIG is necessary for older children with Kawasaki disease (KD), because they could have more complications and financial burden. The purpose of this study was to compare outcomes between high- and low-dose IVIG in KD children with higher body weight (25 kg or more), using a national inpatient database in Japan from 2010 to 2017. We identified those receiving 2-g/kg and 1-g/kg IVIG as an initial treatment. Outcomes included the proportions of coronary artery abnormality (CAA) formation, IVIG resistance, adverse effects, length of stay, and medical costs. A propensity score matching analysis was conducted to compare the outcomes between the groups. We identified 1332 patients with KD and created 4:1 propensity score-matched pairs between high- and low-dose IVIG groups. There were no significant differences in the proportions of CAA (5.3% vs. 4.1%; p = 0.587), IVIG resistance, and length of stay. Medical costs were significantly higher in the high-dose group than in the low-dose group (p < 0.001).Conclusion: No significant difference was shown between the high- and low-dose IVIG groups in the proportions of outcomes, while medical costs were higher in the high-dose group. Further studies are needed to ascertain the appropriate IVIG dose in older patients with KD. What is Known: • For treatments of Kawasaki disease at any age in the acute phase, 2-g/kg single-dose intravenous immunoglobulin and aspirin have been the most recommended to reduce fever early and prevent complications of coronary artery abnormalities. What is New: • There was no significant difference in outcomes between children with Kawasaki disease weighing ≥ 25 kg treated with high-dose or low-dose IVIG in terms of coronary artery abnormalities, IVIG resistance, adverse effects, and length of stay, except for medical costs.
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http://dx.doi.org/10.1007/s00431-020-03794-2DOI Listing
December 2020

Flexible C-C Bonds: Reversible Expansion, Contraction, Formation, and Scission of Extremely Elongated Single Bonds.

Angew Chem Int Ed Engl 2020 Dec 30;59(49):22252-22257. Epub 2020 Sep 30.

Department of Chemistry, Faculty of Science, Hokkaido University, Sapporo, 060-0810, Japan.

Since carbon-carbon (C-C) covalent bonds are rigid and robust, the bond length is, in general, nearly constant and depends only on the bond order and hybrid orbitals. We report herein direct visualization of the reversible expansion and contraction of a C(sp )-C(sp ) single bond by light and heat. This flexibility of a C-C bond was demonstrated by X-ray analysis and Raman spectroscopy of hexaphenylethane (HPE)-type hydrocarbons with two spiro-dibenzocycloheptatriene units, the intramolecular [2+2] photocyclization of which and thermal cleavage of the resulting cyclobutane ring both occur in a single-crystalline phase. The force constant of the contracted C-C bond is 1.6 times greater than that of the expanded bond. Since formation of the cyclobutane ring and contraction of the C-C bond lower the HOMO level by approximately 1 eV, the oxidative properties of these HPEs with a flexible C-C bond can be deactivated/activated by light/heat.
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http://dx.doi.org/10.1002/anie.202010615DOI Listing
December 2020

Senescence-associated secretory phenotype promotes chronic ocular graft-vs-host disease in mice and humans.

FASEB J 2020 08 3;34(8):10778-10800. Epub 2020 Jul 3.

Department of Ophthalmology, Keio University School of Medicine, Tokyo, Japan.

Chronic graft-vs-host disease (cGVHD) is a multifactorial inflammatory disease that affects patients undergoing hematopoietic stem cell transplantation. Multiple organs, including the lacrimal glands (LGs), are negatively affected by cGVHD and lose function due to the resultant fibrosis. An abnormal immune response is thought to be a major factor in the development of chronic ocular GVHD, which is currently treated primarily with immunosuppressive therapies. However, all the treatments yield unsatisfactory outcomes, and additional treatment strategies are needed. To meet this unmet medical need, we aimed to elucidate an additional pathway of chronic ocular GVHD. Our findings suggest a potential association between chronic ocular GVHD pathogenesis and stress-induced cellular senescence through the senescence-associated secretory phenotype (SASP). Senescent cells produce cytokines and chemokines, such as IL-6 and CXCL9. Indeed, senescent cell accumulation was presumably associated with cGVHD development in LGs, as evidenced by the improvement in LGs after the selective elimination of senescent cells (senolysis) with ABT-263. Results in the sclerodermatous cGVHD mouse model suggest that inhibiting the major components of the SASP, including IL-6 and CXCL9, with senolytics is a potential novel strategy for treating cGVHD-affected LGs. Taken together, our results indicate a potential association between the SASP and cGVHD development in LGs and suggest that targeted senolytic treatment may be a new therapeutic option for this disease.
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http://dx.doi.org/10.1096/fj.201900218RDOI Listing
August 2020

Hexaarylbutadiene: A Versatile Scaffold with Tunable Redox Properties towards Organic Near-Infrared Electrochromic Material.

Chem Asian J 2020 Apr 10;15(7):1147-1155. Epub 2020 Mar 10.

Department of Chemisry, Faculty of Science, Hokkaido University, N10 W8, North-ward, Sapporo, 060-0810, Japan.

When the 1,1,4,4-tetraanilinobutadiene skeleton is attached with two halogenated aryl units at the 2,3-positions, they undergo facile two-electron oxidation to give stable dicationic dyes which exhibit a near-infrared (NIR) absorption whereas the neutral dienes show only pale color. Therefore, a distinct electrochromic response with an absorption change in the NIR region is achieved, which is attracting considerable recent attention from the viewpoint of bioimaging. Herein, we demonstrate that the redox potentials of the 1,1,4,4-tetraanilinobutadiene can be precisely controlled by the donating properties of the amino group on the aniline unit as well as the number of halogen atoms on the aryl units at 2,3-positions on the butadiene. In contrast, the NIR absorption bands mainly depend on the number of halogen atoms irrespective to the donating properties of aniline unit. Thus, the hexaarylbutadiene skeleton is proven to be a versatile scaffold to develop less-explored organic NIR electrochromic materials, whose redox and spectroscopic properties can be finely tuned by modifying/attaching the proper substituents.
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http://dx.doi.org/10.1002/asia.201901816DOI Listing
April 2020

HS-activatable near-infrared afterglow luminescent probes for sensitive molecular imaging in vivo.

Nat Commun 2020 01 23;11(1):446. Epub 2020 Jan 23.

State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210023, China.

Afterglow luminescent probes with high signal-to-background ratio show promise for in vivo imaging; however, such probes that can be selectively delivered into target sites and switch on afterglow luminescence remain limited. We optimize an organic electrochromic material and integrate it into near-infrared (NIR) photosensitizer (silicon 2,3-naphthalocyanine bis(trihexylsilyloxide) and (poly[2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylenevinylene]) containing nanoparticles, developing an HS-activatable NIR afterglow probe (F1-ANP). F1-ANP displays a fast reaction rate (1563 ± 141 M s) and large afterglow turn-on ratio (~122-fold) toward HS, enabling high-sensitivity and -specificity measurement of HS concentration in bloods from healthy persons, hepatic or colorectal cancer patients. We further construct a hepatic-tumor-targeting and HS-activatable afterglow probe (F1-ANP-Gal) for noninvasive, real-time imaging of tiny subcutaneous HepG2 tumors (<3 mm in diameter) and orthotopic liver tumors in mice. Strikingly, F1-ANP-Gal accurately delineates tumor margins in excised hepatic cancer specimens, which may facilitate intraoperative guidance of hepatic cancer surgery.
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http://dx.doi.org/10.1038/s41467-020-14307-yDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6978336PMC
January 2020

Molecular Wires with Controllable π-Delocalization Incorporating Redox-Triggered π-Conjugated Switching Units.

Chempluschem 2019 06 24;84(6):634-642. Epub 2018 Aug 24.

Department of Chemistry, Faculty of Science, Hokkaido University, Sapporo, 060-0810, Japan.

A perfluorobiphenyl-2,2'-diyl dication and its corresponding dihydrophenanthrene-type electron donor are interconvertible upon two-electron transfer. Redox-triggered C-C bond-formation/cleavage caused a drastic change in the torsion angle of the biphenyl unit. Thus, π-delocalization ON/OFF switching was observed as a change in the UV absorption upon electrolysis of the linearly extended analogue with two phenylethynyl groups. A further extended π-system with a molecular length of ca. 3.5 nm, which has two switching units, was synthesized. Spectroelectrograms as well as voltammetric analyses showed that the two units act nearly simultaneously because of the very small inter-unit electrostatic repulsion in the tetracationic state. Thus, the present pair is a promising candidate as a switching unit for "molecular wires" with controllable π-delocalization, in which a higher ON/OFF ratio of delocalization could be realized by incorporating multiple switching units.
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http://dx.doi.org/10.1002/cplu.201800341DOI Listing
June 2019

Switching of Redox Properties Triggered by a Thermal Equilibrium between Closed-Shell Folded and Open-Shell Twisted Species.

Angew Chem Int Ed Engl 2020 Apr 20;59(16):6581-6584. Epub 2020 Feb 20.

Department of Chemistry, Faculty of Science, Hokkaido University, Sapporo, 060-0810, Japan.

Thermally switchable redox properties have been reported to be due to a change in the spin state of newly designed overcrowded ethylenes, which can adopt closed-shell folded and open-shell twisted forms. In this study, tetrathienylanthraquinodimethane derivatives were designed to be in thermal equilibrium between a more stable folded form and less stable but more donating twisted diradical in solution, so that the oxidation potential can be controlled by heating/cooling. This is the first example of a switching of redox properties based on a thermally equilibrated twisted diradical, which can be more readily oxidized to the twisted dication.
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http://dx.doi.org/10.1002/anie.201916089DOI Listing
April 2020

Electric-Field-Controllable Conductance Switching of an Overcrowded Ethylene Self-Assembled Monolayer.

J Am Chem Soc 2019 Nov 12;141(46):18544-18550. Epub 2019 Nov 12.

Department of Chemistry, Graduate School of Science and Engineering , Tokyo Institute of Technology , 2-12-1 W4-10 Ookayama , Meguro-ku , Tokyo 152-8551 , Japan.

Molecular isomerism has been discussed from the viewpoint of the tiniest switch and memory elements in electronics. Here, we report an overcrowded ethylene-based molecular conductance switch, which fulfills all the essential requirements for implementation into electronic devices, namely, electric-field-controllable reversible conductance change with a molecular-level spatial resolution, robust conformational bistability under ambient conditions, and ordered monolayer formation on electrode surfaces. The conformational state of this overcrowded ethylene, represented by a folded or twisted conformer, is susceptible to external environments. Nanoscopic measurements using scanning tunneling microscopy techniques, together with theoretical simulations, revealed the electronic properties of each conformer adsorbed on Au(111). While the twisted conformer prevails in the molecularly dispersed state, upon self-assembly into a monolayer, a two-dimensional network structure of the folded conformer is preferentially formed due to particular intermolecular interaction. In the monolayer state, folded-to-twisted and its reverse isomerization can be controlled by the modulation of electric fields.
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http://dx.doi.org/10.1021/jacs.9b09233DOI Listing
November 2019

The formation of perinucleolar bodies is important for normal leaf development and requires the zinc-finger DNA-binding motif in Arabidopsis ASYMMETRIC LEAVES2.

Plant J 2020 03 29;101(5):1118-1134. Epub 2019 Nov 29.

Division of Biological Science, Graduate School of Science, Nagoya University, Nagoya, Aichi, 464-8602, Japan.

In Arabidopsis, the ASYMMETRIC LEAVES2 (AS2) protein plays a key role in the formation of flat symmetric leaves via direct repression of the abaxial gene ETT/ARF3. AS2 encodes a plant-specific nuclear protein that contains the AS2/LOB domain, which includes a zinc-finger (ZF) motif that is conserved in the AS2/LOB family. We have shown that AS2 binds to the coding DNA of ETT/ARF3, which requires the ZF motif. AS2 is co-localized with AS1 in perinucleolar bodies (AS2 bodies). To identify the amino acid signals in AS2 required for formation of AS2 bodies and function(s) in leaf formation, we constructed recombinant DNAs that encoded mutant AS2 proteins fused to yellow fluorescent protein. We examined the subcellular localization of these proteins in cells of cotyledons and leaf primordia of transgenic plants and cultured cells. The amino acid signals essential for formation of AS2 bodies were located within and adjacent to the ZF motif. Mutant AS2 that failed to form AS2 bodies also failed to rescue the as2-1 mutation. Our results suggest the importance of the formation of AS2 bodies and the nature of interactions of AS2 with its target DNA and nucleolar factors including NUCLEOLIN1. The partial overlap of AS2 bodies with perinucleolar chromocenters with condensed ribosomal RNA genes implies a correlation between AS2 bodies and the chromatin state. Patterns of AS2 bodies in cells during interphase and mitosis in leaf primordia were distinct from those in cultured cells, suggesting that the formation and distribution of AS2 bodies are developmentally modulated in plants.
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http://dx.doi.org/10.1111/tpj.14579DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7155070PMC
March 2020

Photo- and Thermal Interconversion of Multiconfigurational Strained Hydrocarbons Exhibiting Completely Switchable Oxidation to Stable Dicationic Dyes.

J Am Chem Soc 2019 Nov 1;141(45):18293-18300. Epub 2019 Nov 1.

Department of Chemistry, Faculty of Science , Hokkaido University , Sapporo 060-0810 , Japan.

Highly strained hydrocarbons with two di/tribenzocycloheptatriene units were designed as electrochromic overcrowded ethylenes that undergo reversible interconversion with stable dicationic dyes. Due to severe steric repulsion, two configurational isomers (,-folded and ,-folded forms) were isolated as stable entities. Photo- and thermal interconversion of these isomers proceeded cleanly: one-way photoisomerization occurred from ,- to ,-form and one-way thermal isomerization was observed from ,- to ,-form. Even though both isomers undergo two-electron oxidation into the same twisted dications, quite different oxidation potentials enable completely selective oxidation of ,-isomers. Thus, the present multiconfigurational strained hydrocarbons are capable of switching of activation/deactivation of their electrochromic properties by light/heat.
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http://dx.doi.org/10.1021/jacs.9b09646DOI Listing
November 2019

Perivascular Epithelial Cell Tumor of the Pancreas Diagnosed Preoperatively by Endoscopic Ultrasound-guided Fine-needle Aspiration.

Intern Med 2019 Sep 7;58(17):2515-2521. Epub 2019 Jun 7.

Department of Gastroenterology, Japanese Red Cross Nagoya Daini Hospital, Japan.

We herein report a 49-year-old woman with a perivascular epithelial cell tumor (PEComa) of the pancreas. Imaging studies demonstrated a relatively well-demarcated mass, measuring approximately 40 mm in diameter, located in the pancreatic tail. It was heterogeneously enhanced almost to the same degree as the surrounding pancreatic tissue in both the arterial and portal venous phases. We performed endoscopic ultrasound-guided fine-needle aspiration (EUS-FNA) using the Acquire 22-gauge needle and preoperatively obtained a definitive diagnosis with a sufficient sample. Clinicians should consider pancreatic PEComa in their differential diagnosis of patients with a pancreatic mass.
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http://dx.doi.org/10.2169/internalmedicine.2265-18DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6761333PMC
September 2019

Chiral diversification through the assembly of achiral phenylacetylene macrocycles with a two-fold bridge.

Chem Sci 2019 May 2;10(18):4782-4791. Epub 2019 Apr 2.

Department of Chemistry , Faculty of Science , Hokkaido University , Sapporo 060-0810 , Japan . Email: ; ; Tel: +81 11 706-3396.

We demonstrate so-called "chiral diversification", which is a design strategy to create multiple chiral molecules through the assembly and double-bridging of achiral components. We used phenylacetylene macrocycles (PAMs) as an achiral element. In a molecule, two achiral rings of [6]PAM are stacked one above the other, or bound to each other mechanically. As an alternative, a single enlarged ring of [12]PAM was also assumed to be a doubled form of [6]PAM. In any case, one or two ring(s) are doubly-bridged by covalent bonds to exert chirality. Through intramolecular two-bond formation, these multiple chiral molecules were obtained as a set of products in one reaction. The dynamic chirality generated in molecules with either two helically-stacked rings of [6]PAM or a single helically-folded ring of [12]PAM was characterized by induced Cotton effects with the aid of an external chiral source. Thus, a chiral structure based on [12]PAM could be demonstrated as the first success. Alternatively, enantiomeric separation was achieved for molecules with two interlocked rings of [6]PAM to show remarkable chiroptical properties.
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http://dx.doi.org/10.1039/c9sc00972hDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6510063PMC
May 2019

Dual dynamic chirality generated in the assembly of three achiral rods through the three-fold twisting of a macrocycle.

Chem Commun (Camb) 2019 May;55(38):5503-5506

Department of Chemistry, Faculty of Science, Hokkaido University, Sapporo 060-0810, Japan.

We demonstrated dynamic chirality based on assemblies of three achiral rods with a twisted macrocycle. The three-fold twisting of a macrocycle can lead to two different chiral forms with C2- or D3-symmetry. Through a transmission of chirality to each dynamic chiral form, a helical-sense preference was successfully induced.
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http://dx.doi.org/10.1039/c9cc02226kDOI Listing
May 2019

Selective Formation of a Mixed-Valence State from Linearly Bridged Oligo(aromatic diamines): Drastic Structural Change into a Folded Columnar Stack for Half-filled Polycations.

Chemistry 2019 Jun 13;25(32):7759-7765. Epub 2019 May 13.

Department of Chemistry, Faculty of Science, Hokkaido University, Sapporo, 060-0810, Japan.

A method to obtain an organic mixed-valence state with long-range delocalization is proposed, which enables the selective generation of half-filled (n/2-charged) polycations from linearly bridged oligomers with n electron-donating units. When π-extended phenylenediamine units are connected by meta-xylylene-type spacers, the resulting oligomers adopt non-folded structures in the neutral state owing to the non-conjugating and flexible nature of the spacer, whereas the structure shows a drastic change into a one-dimensional columnar stack upon oxidation to the corresponding half-filled polycations. Although they are nano-sized discrete molecules, they can mimic the electronic structure of crystalline organic conductors in a mixed-valence state. The key for the oligomer design is adoption of the best-matched spacer that facilitates formation of the singly charged pimer in the dichromophoric system whereas the corresponding doubly charged π-dimer is disfavored.
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http://dx.doi.org/10.1002/chem.201901272DOI Listing
June 2019

Effectiveness of antiplatelet therapy for Kawasaki disease: a systematic review.

Eur J Pediatr 2019 Jun 28;178(6):947-955. Epub 2019 Mar 28.

Department of Management and Strategy, Clinical Research Center, National Center for Child Health and Development, Tokyo, Japan.

Kawasaki disease is an acute systemic vasculitis in children. Antiplatelet medicines are commonly used for Kawasaki disease to attenuate vasculitis and prevent thromboembolism; however, the mechanisms have not been elucidated. The objective of this study is to assess the effectiveness of antiplatelet medications for Kawasaki disease. We used Medline, Embase, Cochrane Central Register of Controlled Trials, and Igaku Chuo Zasshi (Ichushi) from January 1947 to August 2018. Studies describing the platelet functions of antiplatelet drugs for Kawasaki disease were included. Twenty studies met the inclusion criteria. There were no randomized controlled trials. Seven studies compared platelet aggregation ability before and after treatment. Eight studies compared platelet aggregation with that in Kawasaki disease patients without treatment. Four studies compared aggregation among different types of antiplatelet drugs or at different doses. Antiplatelet medications administered in the studies included aspirin, flurbiprofen, dipyridamole, and choline salicylate. Methods for the measurement of platelet aggregation ability varied among studies. The groups with antiplatelet treatment tended to have a decreased platelet aggregation function. The statistical analyses were impossible due to insufficient quantitative data and heterogeneity among the studies.Conclusion: The present systematic review revealed that there was insufficient evidence for the effectiveness of antiplatelet therapy for Kawasaki disease. What is Known: • Antiplatelet therapy is widely used for Kawasaki disease to mitigate cardiac complications. • The mechanisms of antiplatelet therapy for Kawasaki disease are not clarified. What is New: • This systematic review showed that the groups with antiplatelet treatment tended to have a decreased platelet aggregation function. • There is insufficient evidence for the effectiveness of antiplatelet therapy for Kawasaki disease.
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http://dx.doi.org/10.1007/s00431-019-03368-xDOI Listing
June 2019

Direct synthesis of aryl-annulated []carbazoles by gold(i)-catalysed cascade reaction of azide-diynes and arenes.

Chem Sci 2018 Nov 10;9(44):8416-8425. Epub 2018 Sep 10.

Graduate School of Pharmaceutical Sciences , Kyoto University , Sakyo-ku , Kyoto 606-8501 , Japan . Email:

The gold-catalysed annulation of conjugated alkynes bearing an azido group with arenes gave annulated []carbazoles. Using benzene, pyrrole, and indole derivatives as the nucleophiles, benzo[]-, pyrrolo[2,3-]-, and indolo[2,3-]carbazoles were produced, respectively. The reaction proceeded through pyrrole and benzene ring construction accompanied by the formation of two carbon-carbon and one carbon-nitrogen bond and the cleavage of two aromatic C-H bonds. The mechanism of the reaction with pyrrole was investigated by density functional theory calculations. ,'-dimethylated indolo[2,3-]carbazole showed dual ultraviolet-visible-near-infrared and fluorescence spectral changes upon electrolysis.
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http://dx.doi.org/10.1039/c8sc03525cDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6244455PMC
November 2018

Engineering of Electrochromic Materials as Activatable Probes for Molecular Imaging and Photodynamic Therapy.

J Am Chem Soc 2018 11 14;140(47):16340-16352. Epub 2018 Nov 14.

State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering , Nanjing University , Nanjing 210023 , China.

Electrochromic materials (EMs) are widely used color-switchable materials, but their applications as stimuli-responsive biomaterials to monitor and control biological processes remain unexplored. This study reports the engineering of an organic π-electron structure-based EM (dicationic 1,1,4,4-tetraarylbutadiene, 1) as a unique hydrogen sulfide (HS)-responsive chromophore amenable to build HS-activatable fluorescent probes (1-semiconducting polymer nanoparticles, 1-SNPs) for in vivo HS detection. We demonstrate that EM 1, with a strong absorption (500-850 nm), efficiently quenches the fluorescence (580, 700, or 830 nm) of different fluorophores within 1-SNPs, while the selective conversion into colorless diene 2 via HS-mediated two-electron reduction significantly recovers fluorescence, allowing for non-invasive imaging of hepatic and tumor HS in mice in real time. Strikingly, EM 1 is further applied to design a near-infrared photosensitizer with tumor-targeting and HS-activatable ability for effective photodynamic therapy (PDT) of HS-related tumors in mice. This study demonstrates promise for applying EMs to build activatable probes for molecular imaging of HS and selective PDT of tumors, which may lead to the development of new EMs capable of detecting and regulating essential biological processes in vivo.
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http://dx.doi.org/10.1021/jacs.8b10176DOI Listing
November 2018

Expandability of a long C-O bond by a scissor effect in acenaphthofuran.

Chem Commun (Camb) 2018 Sep;54(73):10300-10303

Department of Chemistry, Faculty of Science, Hokkaido University, Sapporo 060-0810, Japan.

The angle strain induced by ring annulation on a spiro-type naphthofuran weakens its C(sp3)-O bond at the opposite peri-position and endows expandability, so that quite different bond lengths [1.493(3)-1.526(6) Å] are determined for the elongated C(sp3)-O bond of the corresponding spiro-acenaphthofuran derivative upon X-ray analyses of its pseudopolymorphs.
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http://dx.doi.org/10.1039/c8cc05998eDOI Listing
September 2018

Enhanced circular dichroism at elevated temperatures through complexation-induced transformation of a three-layer cyclophane with dualistic dynamic helicity.

Chem Sci 2018 Feb 23;9(8):2222-2229. Epub 2018 Jan 23.

Department of Chemistry , Faculty of Science , Hokkaido University , Sapporo 060-0810 , Japan . Email: ; ; Tel: +81 11 706 3396.

When two planes stacked one above the other are twisted, they provide a dynamic pair of helical conformations with ()- or ()-helicity. We designed a three-layer cyclophane that consists of two such dynamic pairs: the top and middle planes, and the middle and bottom planes. Hence, several global conformations could be created for the overall molecule, , double-helical forms with a pair with the same helicity [(,) or (,)], and a -like form with a pair with a different helicity (,). These conformations dynamically interconvert to each other in solution. Chiroptical properties were given by the helical-sense preference of the double-helical forms, which was brought about through complexation with a chiral hydrogen-bonding guest. In terms of the conformational energy in a complexed state, when a desirable relationship between double-helical and -like forms was attained, complexation-induced circular dichroism was enhanced at elevated temperatures and decreased at lowered temperatures.
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http://dx.doi.org/10.1039/c7sc05242aDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC5897879PMC
February 2018

A Three-Stage Split-Crest Technique: Case Series of Horizontal Ridge Augmentation in the Atrophic Posterior Mandible.

Int J Periodontics Restorative Dent 2018 July/August;38(4):565–573. Epub 2018 Mar 13.

This paper introduces a three-stage split-crest (TSSC) technique for horizontal ridge augmentation in the atrophic posterior mandible. The first stage consists of splitting the ridge. Following a 3- to 4-week healing interval, the second stage consists of expansion of the cortical plate (without elevating the periosteum) and placement of a bone replacement graft material. After 3 to 4 months of healing, the implants are placed. The advantages of this three-stage technique are increased vascularization to the surgical area, a decrease in procedure complications, and improved implant survival rates. An extended treatment time is the main disadvantage. The purpose of this retrospective case series is to review and discuss a new step-by-step surgical procedure of a TSSC technique using a delayed implant placement protocol. The results, advantages, and limitations were also presented.
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http://dx.doi.org/10.11607/prd.2907DOI Listing
December 2018

Epicrestal and subcrestal placement of platform-switched implants: 18 month-result of a randomized, controlled, split-mouth, prospective clinical trial.

Clin Oral Implants Res 2018 Apr 23;29(4):353-366. Epub 2018 Feb 23.

Bluestone Center for Clinical Research, New York University College of Dentistry, New York, NY, USA.

Objectives: To evaluate the changes in marginal bone levels (MBL) and soft tissue dimension around platform-switched implants with the implant-abutment junction (IAJ) placed at the crest or 1.5-2 mm subcrestally.

Materials And Methods: In all, 96 platform-switched implants were placed in either the posterior maxilla or mandible in 48 partially edentulous patients in a split-mouth study. All implants were provisionally restored after 4-5 months and definitively after 6 months (T6). Radiographic assessment of MBL was assessed at implant placement (T0), T6, 12 months (T12), and 18 months (T18) after placement. Mid-buccal soft tissue and papilla measurements were performed at T6, T12, and T18.

Results: In all, 43 patients with 86 implants completed the study. The T18 examination showed an implant survival rate of 100% in both groups. Analysis showed that MBL varied as a function of IAJ location, which indicated more coronal bone levels with subcrestal (2.39 ± 0.08 mm) than with epicrestal placements (0.88 ± 0.08 mm) (p < .05). Greater average marginal bone loss was found in the subcrestal group (0.40 ± 0.07 mm) compared to the epicrestal group (0.13 ± 0.08 mm) although no statistically significant difference was found at T18 (p > .05). Levels of mid-buccal soft tissue had no significant changes over time, regardless of group (p > .05). There was a significant difference in increase in papilla between T6 and T12 and T18 (p = .005 and .001), but not between T12 and T18 (p = .61). These papilla levels and changes were similar between groups (p > .05).

Conclusions: The MBL changes around platform-switched implants with same geometry were not affected by the epicrestal or subcrestal location of the IAJ. Furthermore, the location of the IAJ did not affect the implant survival and soft tissue dimensions. However, no bone loss was located apical to the IAJ when the implants were placed subcrestally.
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http://dx.doi.org/10.1111/clr.13129DOI Listing
April 2018

Supramolecular chiroptical switching of helical-sense preferences through the two-way intramolecular transmission of a single chiral source.

Org Biomol Chem 2018 02;16(7):1167-1171

Department of Chemistry, Faculty of Science, Hokkaido University, Sapporo 060-0810, Japan.

We demonstrate a chiroptical switching system with a simple molecule. The molecule contains a pair of chromophores of diphenylacetylene that are linked with a diyne bond and arranged to exert exciton coupling in helically folded forms with (M)- or (P)-helicity. A tertiary amide group is attached to each end of the looped molecule. The amide carbonyls were used to capture a ditopic hydrogen-bonding guest. A chiral auxiliary group on the amide nitrogen acted as a chiral handle to control the helical-sense preference of dynamic helical forms of the loop. The helical-sense preference is brought about by an intramolecular transmission of point chirality associated with the loop. The preferred sense was switched upon complexation with an achiral additive through the formation of hydrogen bonds. In both states, before and after complexation, the helical-sense preferences were controlled through two-way transmission of the single chiral source.
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http://dx.doi.org/10.1039/c7ob03057fDOI Listing
February 2018

[A Ruptured Middle Cerebral Artery Dissecting Aneurysm Operation in a 2-Year-Old Boy].

No Shinkei Geka 2018 Jan;46(1):27-34

Department of Neurosurgery, Asahi General Hospital.

We report the case of a ruptured dissecting aneurysm in an infant. A 2-year-old boy suffered sudden headache and nausea. CT scan revealed a subarachnoid hemorrhage, and digital subtraction angiography(DSA)revealed a dissecting aneurysm(3.9mm)at a branch of the right middle cerebral artery(MCA). Eight days after onset, carotid angiography revealed enlargement of the aneurysm(up to 6.8 mm). Right frontotemporal craniotomy and aneurysm trapping with STA-MCA bypass was performed. Two years and two months later, the aneurysm recurred as assessed by magnetic resonance angiography(MRA). DSA revealed the recurrence of the aneurysm(7.8mm)proximal to the previous aneurysm and displayed development of collateral flow through leptomeningeal anastomosis between the branches of the MCA. During the second operation, the aneurysm extended to the artery branch proximal to the previous trapping. Parent artery occlusion without bypass was performed. Postoperative DSA revealed collateral flows through leptomeningeal anastomosis between the branch of the MCA and the branch of anterior cerebral artery. At the 3-year follow-up period, abnormal findings on MRI did not appear and he was healthy without any neurologic abnormalities.
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http://dx.doi.org/10.11477/mf.1436203670DOI Listing
January 2018

Dynamic or undynamic chirality generated by helical arrangement of a shape-persistent ring and rod doubly bridged in a molecule.

Chem Commun (Camb) 2018 Jan;54(7):735-738

Department of Chemistry, Faculty of Science, Hokkaido University, Sapporo 060-0810, Japan.

We synthesized molecular assemblies of a ring and rod that were covalently bound in a molecule. The bridged components were helically arranged in a threaded or unthreaded form to show unique chiroptical properties based on shape-persistent m-phenylacetylene rings with six, five and four units and phenylene-ethynylene rods.
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http://dx.doi.org/10.1039/c7cc09485jDOI Listing
January 2018

Incision Design and Soft Tissue Management to Maintain or Establish an Interproximal Papilla Around Integrated Implants: A Case Series.

Int J Periodontics Restorative Dent 2018 Jan/Feb;38(1):61-69

Maintenance or reconstruction of interproximal papilla for a successful dental implant restoration can be challenging. To date, the results from various surgical and prosthetic techniques to maintain or regenerate papilla adjacent to dental implants have been unpredictable. To maintain the quality of the soft tissue around an implant, the blood supply must be preserved and formation of scar tissue must be minimized during surgery. Therefore, incision design is vital to producing an esthetic and successful dental implant restoration. In this study, specific incision designs and soft tissue management techniques were used to preserve or create interproximal papilla around single or adjacent implants.
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http://dx.doi.org/10.11607/prd.2978DOI Listing
October 2018