Publications by authors named "Takeshi Matsumoto"

275 Publications

Association of Sleep Disordered Breathing and Blood Pressure with Albuminuria: The Nagahama Study.

Ann Am Thorac Soc 2021 Aug 4. Epub 2021 Aug 4.

Graduate School of Medicine, Kyoto University, Respiratory Care and Sleep Control Medicine, Kyoto, Japan;

Rationale: Although sleep disordered breathing (SDB) may increase urinary albumin excretion (UAE) by raising nocturnal blood pressure (BP) in addition to diurnal BP, the correlation has not been investigated in a general population.

Objectives: To evaluate the relationships among UAE, SDB and BP during sleep in a large population cohort.

Methods: Among 9,850 community residents, UAE was assessed by the urinary albumin creatinine ratio (UACR) in spot urine. Sleep duration and SDB were evaluated by a wearable actigraph and pulse oximeter, respectively. We calculated the actigraphy-modified 3% oxygen desaturation index (Acti-3%ODI) by correcting the time measured by pulse oximetry according to sleep duration obtained by actigraphy. Further, participants were instructed to measure morning and sleep BP at home by a timer-equipped oscillometric device.

Results: Measurements of sleep parameters, UAE and office BP were completed in 6,568 participants. The multivariate analysis that included confounders showed a significant association of Acti-3%ODI with UACR. (β=0.06, p<0.001) Further, a positive interaction between office systolic BP (SBP) and Acti-3%ODI for UACR was found. (β=0.06, p<0.001) Among the 6,568 persons enrolled in the analysis, 5,313 completed measurements of BP at home. In this cohort, the association of Acti-3%ODI with UACR remained significant (β=0.06, p<0.001) even after morning and sleep SBP were included in the analysis. Further, mediation analysis revealed that 28.3% (95% confidence interval: 14.9-41.7%, p<0.001) of the association of Acti-3%ODI with UACR was explained by the mediation of morning and sleep SBP metrics.

Conclusions: SDB and office SBP were independently and synergistically associated with UAE, which is considered as a risk factor for chronic kidney disease and cardiovascular events. SDB may raise UAE not only by increasing BP but involving other pathologic pathways.
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http://dx.doi.org/10.1513/AnnalsATS.202105-528OCDOI Listing
August 2021

Endovascular Treatment for Lower-extremity Arterial Thrombosis in a Patient with Congenital Afibrinogenemia and a History of Bleeding Complications.

Intern Med 2021 Jul 30. Epub 2021 Jul 30.

Department of Cardiology and Nephrology, Mie University Graduate School of Medicine, Japan.

Congenital afibrinogenemia is a rare autosomal recessive blood disorder that accompanies thrombotic complications and is associated with bleeding tendency. The management of these opposing complications remains a challenge. Endovascular treatment (EVT) for peripheral arterial thrombosis has not been described in previous studies. A 57-year-old man with congenital afibrinogenemia developed back pain and left lower leg pain. The cause of the pain was confirmed to be renal infarction and lower extremity arterial thrombosis by Doppler ultrasound and contrast-enhanced computed tomography. He was treated with EVT for the lower extremity arterial thrombosis, leading to an excellent short-term improvement without bleeding.
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http://dx.doi.org/10.2169/internalmedicine.7542-21DOI Listing
July 2021

Markers of cardiovascular disease risk in sleep-disordered breathing with or without comorbidities: the Nagahama Study.

J Clin Sleep Med 2021 Jun 21. Epub 2021 Jun 21.

Department of Respiratory Care and Sleep Control Medicine, Graduate School of Medicine, Kyoto University, Kyoto, Japan.

Study Objectives: Whether the association between sleep-disordered breathing (SDB) and cardiovascular disease (CVD) is independent of comorbid risk factors for CVD is controversial. The objective of this study is to elucidate whether the association between SDB severity and the surrogate markers of CVD evets differs in relation to the number of comorbidities.

Methods: This cross-sectional study included 7731 participants. Severity of SDB was determined by the oxygen desaturation index adjusted by actigraph-measured objective sleep time. Participants were stratified according to SDB severity and the number of comorbidities (hypertension, diabetes, dyslipidemia and obesity), and the associations between the maximum value of intima-media thickness of the common carotid artery (CCA-IMT-max), brachial-ankle pulse wave velocity (baPWV) and cardio-ankle vascular index (CAVI) were evaluated.

Results: Among participants with no risk factor, CCA-IMT-max increased according to SDB severity (n = 1022, <0.0001). Even after the matching of background, the median CCA-IMT-max value was 14% higher in moderate-severe SDB cases than those without SDB (n=45 in each group, =0.020). The difference was not significant for baPWV and CAVI. On the other hand, a significant difference in CCA-IMT-max was not found in those with multiple comorbidities. Consistently, multiple regression analysis revealed an independent association between CCA-IMT-max and moderate-severe SDB for all study participants (β: 0.0222 (95% confidence interval: 0.0039-0.0405), =0.017), but the association was not significant for stratified participants with multiple comorbidities.

Conclusions: SDB severity is associated with the CCA-IMT-max level, but the independent association becomes weaker for those with multiple comorbidities.
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http://dx.doi.org/10.5664/jcsm.9460DOI Listing
June 2021

The Evaluation of Hemostatic Abnormalities Using a CWA-Small Amount Tissue Factor Induced FIX Activation Assay in Major Orthopedic Surgery Patients.

Clin Appl Thromb Hemost 2021 Jan-Dec;27:10760296211012094

Department of Orthopaedic Surgery, Mie University Graduate School of Medicine, Tsu, Japan.

We analyzed the utility for a clot waveform analysis (CWA) of small tissue factor induced FIX activation (sTF/FIXa) assay in patients with major orthopedic surgery (including total hip arthroplasty [THA] and total knee arthroplasty [TKA]) receiving edoxaban for the prevention of venous thromboembolism (VTE). The sTF/FIXa assay using recombinant human TF in platelet-rich plasma (PRP) and platelet-poor plasma (PPP) was performed using a CWA in the above patients to monitor the efficacy of edoxaban administration. Of 147 patients (109 THA and 38 TKA), 21 exhibited deep vein thrombosis (DVT), and 15 had massive bleeding. Increased peak heights of the CWA-sTF/FIX were observed in almost patients after surgery and prolonged peak heights of the CWA-sTF/FIX were observed in almost patients treated with edoxaban. The peak heights and times of the CWA-sTF/FIX were significantly higher and shorter, respectively, in PRP than in PPP. There were no significant differences in parameters of the CWA-sTF/FIXa between the patients with and without DVT or between those with and without massive bleeding. The peak time of CWA-sTF/FIXa were significantly longer in TKA patients than in THA patients on day 1 after surgery. The second derivative peak height of the CWA-sTF/FIXa was significantly lower in TKA patients than in THA patients on day 4. The CWA-sTF/FIX reflected hemostatic abnormalities after surgery and the administration of edoxaban, and the results were better in PRP than PPP. Further studies separately analyzing the THA and TKA subgroups should be conducted.
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http://dx.doi.org/10.1177/10760296211012094DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8150457PMC
May 2021

A Liposomal Gemcitabine, FF-10832, Improves Plasma Stability, Tumor Targeting, and Antitumor Efficacy of Gemcitabine in Pancreatic Cancer Xenograft Models.

Pharm Res 2021 Jun 7;38(6):1093-1106. Epub 2021 May 7.

Bioscience and Engineering laboratories, FUJIFILM Corporation, 577 Ushijima, Kaisei-machi, Ashigarakami-gun, Kanagawa, 258-8577, Japan.

Purpose: The clinical application of gemcitabine (GEM) is limited by its pharmacokinetic properties. The aim of this study was to characterize the stability in circulating plasma, tumor targeting, and payload release of liposome-encapsulated GEM, FF-10832.

Methods: Antitumor activity was assessed in xenograft mouse models of human pancreatic cancer. The pharmacokinetics of GEM and its active metabolite dFdCTP were also evaluated.

Results: In mice with Capan-1 tumors, the dose-normalized areas under the curve (AUCs) after FF-10832 administration in plasma and tumor were 672 and 1047 times higher, respectively, than after using unencapsulated GEM. The tumor-to-bone marrow AUC ratio of dFdCTP was approximately eight times higher after FF-10832 administration than after GEM administration. These results indicated that liposomal encapsulation produced long-term stability in circulating plasma and tumor-selective targeting of GEM. In mice with Capan-1, SUIT-2, and BxPC-3 tumors, FF-10832 had better antitumor activity and tolerability than GEM. Internalization of FF-10832 in tumor-associated macrophages (TAMs) was revealed by flow cytometry and confocal laser scanning microscopy, and GEM was efficiently released from isolated macrophages of mice treated with FF-10832. These results suggest that TAMs are one of the potential reservoirs of GEM in tumors.

Conclusion: This study found that FF-10832 had favorable pharmacokinetic properties. The liposomal formulation was more effective and tolerable than unencapsulated GEM in mouse xenograft tumor models. Hence, FF-10832 is a promising candidate for the treatment of pancreatic cancer.
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http://dx.doi.org/10.1007/s11095-021-03045-5DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8217058PMC
June 2021

Evaluation of hemostatic abnormalities in patients who underwent major hepatobiliary pancreatic surgery using activated partial thromboplastin time-clot waveform analysis.

Thromb Res 2021 05 9;201:154-160. Epub 2021 Apr 9.

Department of Hepatobiliary Pancreatic and Transplant Surgery, Mie University Graduate School of Medicine, 174-2 Edobashi, Tsu, Mie, Japan.

Introduction: Bleeding after major hepatobiliary pancreatic (HBP) surgery may be serious. Although postoperative abnormality of the hemostatic system are important elements that affect bleeding, routine activated partial thromboplastin time (APTT) assessment is considered inadequate to predict massive bleeding (MB). Recently, APTT-clot waveform analysis (CWA) was reported to be useful for detecting coagulation disorders.

Methods: APTT-CWA was performed using the ACL-TOP analyzer in 188 patients who underwent four major HBP surgeries (distal pancreatectomy, hepatectomy, subtotal stomach-preserving pancreatoduodenectomy (SSPPD), and SSPPD with combined resection and reconstruction of the portal vein) to analyze its usefulness in predicting the risk of bleeding.

Results: Seventy (37.2%) patients developed MB and the incidence of MB was highest among patients who underwent hepatectomy. There were no significant differences in routine APTT, the first derivative peak (DP) time and 1/2 fibrin formation peak time between patients with MB and those without MB, throughout the postoperative course. On the other hand, the first and second DP heights were significantly lower in patients with MB than in those without MB and lowest in patients who underwent hepatectomy.

Conclusion: APTT-CWA was able to detect the detailed changes in the hemostatic system after major HBP surgery. The patterns of APTT-CWA after major HBP surgery differed among various surgical procedures according to invasiveness. The lower first and the second DP height, which were frequently observed in hepatectomy patients, may be useful for predicting the risk of MB.
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http://dx.doi.org/10.1016/j.thromres.2021.03.030DOI Listing
May 2021

[Successful treatment with cyclosporine in a patient with rituximab-refractory thrombocytopenic purpura].

Rinsho Ketsueki 2021 ;62(3):176-179

Department of Hematology and Oncology, Mie University Hospital.

Acquired thrombotic thrombocytopenic purpura (aTTP) is a life-threatening systemic thrombotic microangiopathy characterized by the presence of anti-ADAMTS13 antibodies (inhibitor). Here we report the case of a patient with refractory aTTP successfully treated with cyclosporine. A 69-year-old man presenting with hematuria and petechiae was referred to our hospital; he was disoriented and febrile. Laboratory results revealed Coombs-negative hemolytic anemia, thrombocytopenia, and renal failure. Undetectable ADAMTS13 activity and presence of anti-ADAMTS13 antibodies (inhibitor) confirmed the diagnosis of aTTP. Despite performing plasma exchange and administering prednisolone and rituximab (375 mg/m), we were unable to restore his platelet counts to the normal level. Therefore, he was treated with cyclophosphamide (500 mg/bodyweight), vincristine (1.4 mg/m), bortezomib (1.3 mg/m), and cyclosporine (2.5 mg/kg). After the cyclosporine therapy, his platelet counts gradually normalized. Continuous cyclosporine maintenance therapy led to complete disappearance of the inhibitor. Therapeutic strategies for refractory aTTP have not yet been established. Further investigations are warranted to establish a therapeutic strategy for refractory aTTP.
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http://dx.doi.org/10.11406/rinketsu.62.176DOI Listing
April 2021

Useful Parameters in Dynamic Contrast-enhanced Ultrasonography for Identifying Early Response to Chemotherapy in a Rat Liver Tumor Model.

J Clin Imaging Sci 2021 15;11:15. Epub 2021 Mar 15.

Department of Radiology, Nara Medical University, Kashihara, Nara, Japan.

Objectives: The objective of the study is to determine a parameter on the time-intensity curve (TIC) of dynamic contrast-enhanced ultrasonography (DCE-US) that best correlates with tumor growth and to evaluate whether the parameter could correlate with the early response to irinotecan in a rat liver tumor model.

Material And Methods: Twenty rats with tumors were evaluated (control: Saline, = 6; treatment: Irinotecan, = 14) regarding four parameters from TIC: Peak intensity (PI), k value, slope (PI × k), and time to peak (TTP). Relative changes in maximum tumor diameter between day 0 and 10, and parameters in the first 3 days were evaluated. The Mann-Whitney U-test was used to compare differences in tumor size and other parameters. Pearson's correlation coefficients (r) between tumor size and parameters in the control group were calculated. In the treatment group, relative changes of parameters in the first 3 days were compared between responder and non-responder (<20% and ≥20% increase in size on day 10, respectively).

Results: PI, k value, PI × k, and TTP significantly correlated with tumor growth ( = 0.513, 0.911, 0.665, and 0.741, respectively). The mean RC in k value among responders ( = 6) was significantly lower than non-responders ( = 8) (mean k value, 4.96 vs. 72.5; = 0.003).

Conclusion: Parameters of DCE-US could be a useful parameter for identifying early response to irinotecan.
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http://dx.doi.org/10.25259/JCIS_6_2020DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7981939PMC
March 2021

Characteristics of patients with frequent systemic corticosteroid bursts for asthma in real clinical practice: are there frequent "short bursts?"

J Asthma 2021 Apr 1:1-8. Epub 2021 Apr 1.

Department of Respiratory Medicine, Saiseikai-Noe Hospital, Osaka, Japan.

Objective: The data on intermittent systemic corticosteroid therapy for asthma exacerbation, clinically called a "short burst," is limited. This study aimed to investigate the characteristics of patients with frequent systemic corticosteroid bursts for asthma in real clinical practice.

Methods: Consecutive patients who regularly visited our hospital for asthma treatment between January 2019 and December 2020 were reviewed. The number of systemic corticosteroid bursts during the past 1 year was collected, and those with frequent bursts (≥2 times/year) were defined as the Frequent group.

Results: Data on 236 patients were analyzed. Among them, 5.5% (95% confidence interval 3.2-9.2%) were in the Frequent group. In the Frequent group, 23% of patients had no unplanned visits, and 38% experienced at least one corticosteroid burst without visiting a physician (self-medication). One-third of patients did not undertake high-dose inhaled corticosteroid treatment, and three-fourths of patients did not undertake long-acting muscarinic antagonist treatment. Low pulmonary function and increased blood eosinophils were independently associated with the Frequent group (adjusted odds ratio = 0.73, 95% confidence interval 0.55-0.99,  = 0.039, per 10% predicted increase in a forced expiratory volume in 1 s; adjusted odds ratio = 1.15, 95% confidence interval 1.02-1.29,  = 0.025, per 100/μL increase in blood eosinophils).

Conclusions: There was a certain rate of frequent corticosteroid bursts in real clinical practice. It is important to determine the actual condition, as some patients experienced "hidden" frequent bursts and have the option to reinforce the treatment.
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http://dx.doi.org/10.1080/02770903.2021.1908350DOI Listing
April 2021

Feasibility and Techniques of Securing 3D-Safety Margin in Superselective Transarterial Chemoembolization to Improve Local Tumor Control for Small Hepatocellular Carcinoma: An Intend-to-Treat Analysis.

Liver Cancer 2021 Feb 12;10(1):63-71. Epub 2021 Jan 12.

Department of Radiology, Nara Medical University, Kashihara, Japan.

Introduction: The aim of this study was to investigate the technical success rate of obtaining 3D-safety margin in superselective conventional transarterial chemoembolization (cTACE) using 3D images for small hepatocellular carcinoma (HCC).

Methods: Consecutive 48 HCC nodules (diameter, 1-3 cm) in 44 patients were intentionally treated by superselective cTACE in an attempt to achieve 3D-safety margin. Superselective CT during hepatic arteriography (CTHA) was obtained before cTACE. When negative 3D-safety margin was found, branches supplied into the margin area were detected by using a 3D workstation. The technical success rate to obtain 3D-safety margin was investigated by intend-to-treat analysis. Local tumor recurrence rate and adverse events were also evaluated.

Result: Nine of 48 tumors (18.8%) had 3D-safety margin in the initial superselective CTHA. After pulling back of the catheter and/or selection of another branch based on 3D images, 3D-safety margin was finally achieved in 45 (93.8%). There were 8 of 46 tumors (17.4%) with local recurrence after 5-year follow-up. Grade 3-4 of aspartate aminotransferase, alanine aminotransferase, and total bilirubin were found in 38.6, 36.4, and 2.3%, respectively. One portal vein thrombus and 3 biliary dilation or biloma were developed.

Conclusion: Superselective cTACE obtaining 3D-safety margin in small HCC was feasible with a high success rate by using 3D images, which could be tolerable and prevent local tumor recurrence.
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http://dx.doi.org/10.1159/000512337DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7923884PMC
February 2021

Early central nervous system relapse of monomorphic epitheliotropic intestinal T-cell lymphoma after cord blood transplantation.

Int J Hematol 2021 Jul 1;114(1):129-135. Epub 2021 Mar 1.

Department of Hematology and Oncology, Mie University Graduate School of Medicine, 2-174 Edobashi, Tsu, Mie, 514-8507, Japan.

Monomorphic epitheliotropic intestinal T-cell lymphoma (MEITL) is a rare subtype of intestinal T-cell lymphoma that occurs mostly in Asia. CHOP-like therapy is usually selected, but the prognosis is very poor. This report concerns a 43-year-old woman with newly diagnosed stage IVA MEITL. The patient obtained a partial response after 4 cycles of GDP (gemcitabine, dexamethasone, cisplatin) and achieved a complete response (CR) after cord blood transplantation (CBT) conditioned with total body irradiation, cyclophosphamide, and cytarabine. Seven months after transplantation, the patient experienced cognitive impairment. Magnetic resonance imaging of the brain showed a high-intensity lesion in the right cerebral peduncle and internal capsule. A cerebrospinal fluid examination confirmed central nervous system (CNS) relapse of MEITL. After 3 cycles of MPV (methotrexate, procarbazine, vincristine) followed by whole-brain radiotherapy, her cognitive impairment improved. Due to disease progression, she died 6 months after CNS relapse. Given the CNS relapse after achieving a CR with GDP and CBT in this patient, CNS prophylaxis during first-line therapy may be beneficial in the treatment of MEITL.
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http://dx.doi.org/10.1007/s12185-021-03107-9DOI Listing
July 2021

Helicobacter pylori type 4 secretion systems as gastroduodenal disease markers.

Sci Rep 2021 Feb 25;11(1):4584. Epub 2021 Feb 25.

Department of Environmental and Preventive Medicine, Faculty of Medicine, Oita University, Yufu, 879-5593, Japan.

Although the type 4 secretion system of the integrating and conjugative elements (tfs ICE) is common in Helicobacter pylori, its clinical association with the cag pathogenicity island (cagPAI) have not yet been well-investigated. In this study, Vietnamese patient H. pylori samples (46 duodenal ulcer (DU), 51 non-cardia gastric cancer (NCGC), 39 chronic gastritis (CG)) were fully sequenced using next-generation sequencing and assembled into contigs. tfs3, tfs4, and cagPAI genes were compared with the public database. Most (94%) H. pylori strains possessed a complete cagPAI, which was the greatest risk factor for clinical outcomes, while the prevalences of tfs3 and tfs4 were 45% and 77%, respectively. Complete tfs3 and tfs4 were found in 18.3% and 17.6% of strains, respectively. The prevalence of H. pylori strains with complete tfs3 ICE in DU patients was significantly higher than that in NCGC patients (30.4% vs 11.7%, P < 0.05). In addition, the prevalence of strains with complete tfs3 ICE and cagPAI was significantly higher in DU patients than that in NCGC (28.4% vs 9.8%, P = 0.038) and CG patients (28.2% vs 7.7%, P = 0.024). cagPAI and complete tfs3 increased the risk of DU compared to NCGC (OR = 3.56, 95%CI: 1.1-14.1, P = 0.038) and CG (OR = 4.64, 95%CI: 1.1-27.6, P = 0.024). A complete cluster of tfs3 ICE was associated with gastroduodenal diseases in Vietnam. However, there was a low prevalence of the dupA/complete dupA cluster (15.4%) in the Vietnam strains. The prevalence of cagPAI in Vietnam strains was significantly higher than in US (P = 0.01) and Indonesia (P < 0.0001); the prevalence of the dupA cluster was also higher in the Vietnam strains than in the Indonesian strains (P < 0.05). In addition, the prevalence of ctkA, an accessory gene of tfs3, was significantly different between Vietnam and US strains (28% vs 2%, P = 0.0002). In summary, the acquisition of tfs3/4 ICE was common in H. pylori strains in patients with gastroduodenal disease in Vietnam, and the complete cluster of tfs3 ICE was a reliable marker for the severity of disease in the H. pylori infected population.
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http://dx.doi.org/10.1038/s41598-021-83862-1DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7907105PMC
February 2021

The Evaluation of APTT Reagents in Reference Plasma, Recombinant FVIII Products; Kovaltry® and Jivi® Using CWA, Including sTF/7FIX Assay.

Clin Appl Thromb Hemost 2021 Jan-Dec;27:1076029620976913

Department of Molecular Pathobiology and Cell Adhesion Biology, Mie University Graduate School of medicine, Tsu, Japan.

The FVIII activity in patients treated with several extended half-life FVIII (EHL-FVIII) agents different when various activated partial thromboplastin time (APTT) reagents were used. The present study examined the difference in clot waveform analysis (CWA) findings and FVIII activity when various APTT reagents and CWA were used. The CWA including FVIII activity was measured using 12 APTT reagents, and the FIX activation based on a small amount of tissue factor assay (sTF/FIX) were examined in reference plasma (RP), EHL-FVIII (Jivi) and Kovaltry. The 3 APTT reagents were associated with high variation in the peak time and height in the CWA when analyzing low concentrations of FVIII. The peak time and height could not be measured with one APTT reagent, and there were marked differences in the CWA findings between Jivi and Kovaltry among APTT reagents. Several APTT reagents showed a markedly lower FVIII activity with Jivi than with Kovaltry. In the FVIII assay, the peak time measured with sTF/FIX did not differ markedly between Jivi and Kovaltry; however, the FVIII activity in Jivi (as measured by the peak height) tended to be higher than in Kovaltry. The CWA findings for monitoring Jivi varied for monitoring Jivi depending on the APTT reagents used, and sTF/FIX assay may be able to measure the EHL-FVIII.
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http://dx.doi.org/10.1177/1076029620976913DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7900842PMC
February 2021

Porphyromonas gingivalis lipopolysaccharide induces interleukin-6 and c-c motif chemokine ligand 2 expression in cultured hCMEC/D3 human brain microvascular endothelial cells.

Gerodontology 2021 Feb 18. Epub 2021 Feb 18.

Department of Vascular Biology, Institute of Brain Science, Hirosaki University Graduate School of Medicine, Hirosaki, Japan.

Objective: This paper describes the effect of Porphyromonas gingivalis (P gingivalis) lipopolysaccharide (LPS) on the expression of interleukin-6 (IL-6) and C-C motif chemokine ligand 2 (CCL2) in cultured hCMEC/D3 human brain microvascular endothelial cells.

Background: P gingivalis is one of the important pathogens in periodontitis, and periodontitis is a risk factor for brain disorders including cerebrovascular diseases and Alzheimer's disease. However, the mechanisms underlying the pathogenesis of P gingivalis-mediated brain diseases are incompletely understood. Effects of P gingivalis LPS on brain endothelial cells are not known well.

Methods: The hCMEC/D3 human brain microvascular endothelial cells were cultured and treated with P gingivalis LPS. The expression of IL-6 and CCL2 mRNA and protein was examined using quantitative reverse transcription-polymerase chain reaction and enzyme-linked immunosorbent assay, respectively. Effect of inhibitors of Toll-like receptor (TLR) 2, TLR4, nuclear factor-κB (NF-κB), p38 mitogen-activated protein kinase (MAPK) and c-Jun N-terminal kinase (JNK) was also investigated. Phosphorylation of NF-κB p65, p38 MAPK and JNK was examined using Western blotting.

Results: P gingivalis LPS-induced mRNA and protein expression of IL-6 and CCL2 in hCMEC/D3 cells in a concentration-dependent manner at the concentration of 0.5-50 µg/mL. Maximal mRNA expression of IL-6 and CCL2 was found 2 and 4 hours after stimulation, respectively. Induction of IL-6 and CCL2 by P gingivalis LPS was almost completely inhibited by pretreatment of cells with TLR4 inhibitor but not by TLR2 inhibitor. Treatment of cells with P gingivalis LPS for up to 2 hours induced phosphorylation of NF-κB p65, p38 MAPK and JNK. IL-6 induction was decreased by pretreatment of cells with NF-κB inhibitor SN50 or p38 MAPK inhibitor SB203580, while CCL2 induction was reduced by SN50 or JNK inhibitor SP600125.

Conclusions: IL-6 and CCL2 produced upon P gingivalis LPS stimulation may contribute to the inflammatory reactions in brain endothelial cells and subsequent neurological disorders such as cerebrovascular and Alzheimer's diseases.
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http://dx.doi.org/10.1111/ger.12545DOI Listing
February 2021

Drastically Progressive Ethambutol-induced Optic Neuropathy after Withdrawal of Ethambutol: A Case Report and Literature Review.

Intern Med 2021 Jun 29;60(11):1785-1788. Epub 2020 Dec 29.

Department of Respiratory Medicine, Saiseikai-Noe Hospital, Japan.

Ethambutol-induced optic neuropathy (EON) is a well-known complication, although low-dose ethambutol seldom causes EON. An 85-year-old man with non-tuberculous mycobacterial lung disease was taking antibiotics, including low-dose ethambutol. On day 85 of treatment, the diagnosis of EON was made. Despite prior discontinuation, his best corrected visual acuity drastically deteriorated from 20/17 (right eye) and 20/20 (left eye) to 20/330 (right eye) and 20/1,000 (left eye) within 3 weeks, and this symptom did not resolve. To our knowledge, there have been no reported cases with drastically progressing and irreversible EON even after the withdrawal of low-dose and short-term ethambutol.
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http://dx.doi.org/10.2169/internalmedicine.6178-20DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8222132PMC
June 2021

Accuracy of an automated method of 3D soft tissue landmark detection.

Eur J Orthod 2020 Dec 26. Epub 2020 Dec 26.

Department of Orthodontics, University of Adelaide, Adelaide, South Australia, Australia.

Introduction: Due to technological advances, the quantification of facial form can now be done via three-dimensional (3D) photographic systems such as stereophotogrammetry. To enable comparison with traditional cephalometry, soft-tissue anatomical landmark definitions have been modified to incorporate the third dimension. Annotating these landmarks manually, however, is still a time-consuming and arduous process.

Objective: To develop an automated algorithm to accurately identify anatomical landmarks on three-dimensional soft tissue images.

Methods: Thirty 3dMD images were selected from a private orthodontic practice consisting of 15 males and 15 females between 9 and 17 years of age. The soft-tissue 3D images were aligned along a reference plane to setup a Cartesian coordinate system. Screened by 2 observers, 21 landmarks were manually annotated and their coordinates defined. An automated landmark identification algorithm, based on their anatomical definitions, was developed to compare the landmark validity against the manually identified counterpart.

Results: Twenty-one landmarks were analysed in detail. Inter-observer and intra-observer reliability using ICC was >0.9. The average difference and standard deviation between manual and automated methods for all landmarks was 3.2 and 1.64 mm, respectively. Sixteen out of twenty-one landmarks had a mean difference less than 4 mm. The landmarks of greatest agreement (≤2 mm) were mainly in the midline: pronasale, subnasale, subspinale, labiale superius, stomion, with the exception of chelion right. Five linear facial measurements were found to have moderate to good agreement between the manual and automated identification methods.

Conclusions: The developed algorithm was determined to be clinically relevant in the detection of midsagittal landmarks and associated measurements within the studied sample of adolescent Caucasian subjects.
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http://dx.doi.org/10.1093/ejo/cjaa069DOI Listing
December 2020

Excited-state hydrogen detachment from a tris-(o-phenylenediamine) iron(ii) complex in THF at room temperature.

Chem Commun (Camb) 2020 Dec 7;56(98):15414-15417. Epub 2020 Dec 7.

Department of Applied Chemistry, Faculty of Science and Engineering, Chuo University, 1-13-27 Kasuga, Bunkyo-ku, Tokyo 112-8551, Japan.

We previously reported that a tris-(o-phenylenediamine) iron(ii) complex promotes photochemical H generation and C-H carboxylation of o-phenylenediamine without any additives under N and CO atmospheres, respectively, in tetrahydrofuran at room temperature. Herein, the key mechanistic process, namely, excited-state hydrogen detachment from the o-phenylendiamine moiety, is demonstrated under an N atmosphere.
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http://dx.doi.org/10.1039/d0cc06219gDOI Listing
December 2020

Ghost chest tube after talc pleurodesis.

Clin Case Rep 2020 Nov 8;8(11):2306-2307. Epub 2020 Jul 8.

Department of Respiratory Medicine Saiseikai-Noe Hospital Osaka Japan.

After the talc pleurodesis, CT showed the tract made from the chest tube even after its removal. The unexpanded thoracic space might also contribute to it; thus, gathering specific medical history is important to understand this rare phenomenon.
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http://dx.doi.org/10.1002/ccr3.3084DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7669413PMC
November 2020

Functional Group-Directed Photochemical Reactions of Aromatic Alcohols, Amines, and Thiols Triggered by Excited-State Hydrogen Detachment: Additive-free Oligomerization, Disulfidation, and C(sp)-H Carboxylation with CO.

J Org Chem 2021 Jan 19;86(1):959-969. Epub 2020 Nov 19.

Department of Applied Chemistry, Faculty of Science and Engineering, Chuo University, 1-13-27 Kasuga, Bunkyo-ku, Tokyo 112-8551, Japan.

Exploring new types of photochemical reactions is of great interest in the field of synthetic chemistry. Although excited-state hydrogen detachment (ESHD) represents a promising prospective template for additive-free photochemical reactions, applications of ESHD in a synthetic context remains scarce. Herein, we demonstrate the expansion of this photochemical reaction toward oligomerization, disulfidation, and regioselective C(sp)-H carboxylation of aromatic alcohols, thiols, and amines. In the absence of any radical initiators in tetrahydrofuran upon irradiation with UV light (λ = 280 or 300 nm) under an atmosphere of N or CO, thiols and catechol afforded disulfides and oligomers, respectively, as main products. Especially, the photochemical disulfidation proceeded highly selectively with the NMR and quantum yields of up to 69 and 0.46%, respectively. In stark contrast, the photolysis of phenylenediamines and aminophenols results in photocarboxylation in the presence of CO (1 atm). -Aminophenol was quantitatively carboxylated by photolysis for 17 h with a quantum yield of 0.45%. Furthermore, the photocarboxylation of phenylenediamines and aminophenols proceeds in a highly selective fashion on the aromatic C(sp)-H bond next to a functional group, which is directed by the site-selective ESHD of the functional groups for the formation of aminyl and hydroxyl radicals.
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http://dx.doi.org/10.1021/acs.joc.0c02456DOI Listing
January 2021

Night-time frequency of urination as a manifestation of sleep-disordered breathing: the Nagahama study.

Sleep Med 2021 01 12;77:288-294. Epub 2020 Sep 12.

Department of Respiratory Care and Sleep Control Medicine, Kyoto University Graduate School of Medicine, Kyoto, Japan.

Aims: Sleep-disordered breathing (SDB) is a well-known risk factor for cardiovascular outcomes. Studies of patients with SDB have identified frequent night-time urination as a manifestation related to SDB. We aimed to clarify whether night-time frequency of urination is independently associated with SDB in a general population. We also investigated whether night-time frequency of urination can help presumptive diagnose SDB.

Methods: Study participants consisted of 7151 community residents. Oxygen saturation during sleep was measured for four nights using a pulse oximeter. SDB was defined as ≥15 events per hour in which oxygen desaturation exceeded or equal to 3% during an actigraphy-determined sleep period. Night-time frequency of urination was recorded for one week using a sleep diary.

Results: Significant positive correlations were evident between night-time frequency of urination and SDB (none, 5.8%; once/night, 14.1%; twice/night, 20.1%; thrice/night, 28.7%; >thrice/night, 44.1%, P < 0.001). This association was independent of possible covariates, including sleep duration (adjusted odds ratio: once/night = 1.50, twice/night = 2.15, thrice/night = 3.07, >thrice/night = 3.73, P < 0.001). Other factors significantly associated with SDB were age, sex, obesity, observation of sleep apnea, and short sleep duration. The area under the curve of the risk score for SDB consisting of these conventional six items (0.834) significantly improved (0.842, P = 0.001) when night-time frequency of urination was considered as a risk score item.

Conclusion: Night-time frequency of urination was associated with SDB. Our findings suggest that the urination frequency should be considered a manifestation of SDB even in a general population.
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http://dx.doi.org/10.1016/j.sleep.2020.09.007DOI Listing
January 2021

Impact of sleep-disordered breathing on glucose metabolism among individuals with a family history of diabetes: the Nagahama study.

J Clin Sleep Med 2021 02;17(2):129-140

Department of Respiratory Care and Sleep Control Medicine, Graduate School of Medicine, Kyoto University, Kyoto, Japan.

Study Objectives: It is well known that a family history of diabetes (FHD) is a definitive risk factor for type 2 diabetes. It has not been known whether sleep-disordered breathing (SDB) increases the prevalence of diabetes in those with an FHD.

Methods: We assessed SDB severity in 7,477 study participants by oximetry corrected by objective sleep duration determined by wrist actigraphy. Glycated hemoglobin ≥6.5% and/or current medication for diabetes indicated the presence of diabetes. In addition to the overall prevalence, the prevalence of recent-onset diabetes during the nearly 5 years before the SDB measurements were made was investigated.

Results: Of the 7,477 participants (mean age: 57.9; range: 34.2-80.7; SD: 12.1 years; 67.7% females), 1,569 had an FHD. The prevalence of diabetes in FHD participants with moderate-to-severe SDB (MS-SDB) was higher than in those without SDB (MS-SDB vs without SDB: all, 29.3% vs 3.3% [P < .001]; females, 32.6% vs 1.9% [P < .001]; males, 26.2% vs 11.7% [P = .037]). However, multivariate analysis showed that MS-SDB was significantly associated with a higher prevalence of diabetes only in FHD-positive females (odds ratio [95% confidence interval]: females, 7.43 [3.16-17.45]; males, 0.92 [0.37-2.31]). Among the FHD-positive participants, the prevalence of recent-onset diabetes was higher in those with MS-SDB than those without SDB, but only in females (MS-SDB vs without SDB: 21.4% vs 1.1%; P < 0.001).

Conclusions: MS-SDB was associated with diabetes risk in females with an FHD, and future studies are needed on whether treatment of SDB in females with an FHD would prevent the onset of diabetes.
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http://dx.doi.org/10.5664/jcsm.8796DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7853232PMC
February 2021

Update on the Clot Waveform Analysis.

Clin Appl Thromb Hemost 2020 Jan-Dec;26:1076029620912027

Department of Molecular Pathobiology and Cell Adhesion Biology, Mie University Graduate School of Medicine, Tsu, Japan.

The activated partial thromboplastin time (APTT)-clot waveform analysis (CWA) was previously reported to be associated with the early detection of disseminated intravascular coagulation and was also reported to be able to measure very low levels of coagulation factor VIII activity. The software program for the analysis for the APTT-CWA allows the associated first and second derivative curves (first and second DCs) to be displayed. The first and second DC reflect the velocity and acceleration, respectively. The height of the first DC reflects the "thrombin burst" and bleeding risk, while that of the second DC is useful for detecting any coagulation factor deficiency and abnormal enhancement of coagulation by phospholipids. Activated partial thromboplastin time-CWA aids in making a differential diagnosis which is difficult to do using only the routine APTT. The CWA is currently used for many applications in the clinical setting, including the monitoring of hemophilia patients and patients receiving anticoagulant therapy and the differential diagnosis of diseases.
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http://dx.doi.org/10.1177/1076029620912027DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7466886PMC
June 2021

Comparison of embolic effect between water-in-oil emulsion and microspheres in transarterial embolization for rat hepatocellular carcinoma model.

Hepatol Res 2020 Nov 7;50(11):1297-1305. Epub 2020 Sep 7.

Department of Radiology, Nara Medical University, Kashihara, Japan.

Aim: To compare two different embolic materials, water-in-oil (W/O) emulsion followed by gelatin particles and microspheres in transarterial embolization (TAE), using a rat hepatocellular carcinoma model.

Methods: Twenty rats bearing N1S1 cells were divided into the W/O emulsion group and Microsphere group. Water-in-oil emulsion was created by a glass membrane emulsification device. The tumor vascularity was measured by contrast-enhanced ultrasonography 24 h before and 10 min and 48 h after TAE. Tumor necrosis, hepatic infarction ratio surrounding the tumor, and locations of the embolic materials 48 h after TAE were assessed. The changes of serum liver enzymes were also evaluated. Statistical significance was determined by using either the Mann-Whitney U-test or Fisher's exact test.

Results: The tumor vascularity 48 h after TAE was significantly higher in the Microsphere group (20.1 vs. 3.76%, P = 0.016). The overflow of Lipiodol into the portal veins surrounding the tumor was seen, whereas microspheres were seen only in the artery. The percentage of necrotic area and complete response ratio in the W/O emulsion group was significantly higher (99.9 vs. 87.6%, P = 0.029 and 87.5 vs. 28.6%, P = 0.041, respectively). Serum aspartate aminotransferase and serum alanine aminotransferase levels 48 h after TAE were significantly higher in the W/O emulsion group (P < 0.01).

Conclusions: The embolization using W/O emulsion followed by gelatin particles showed stronger antitumor effects with the occlusion of both the tumor feeding artery and the portal vein compared with microspheres, which occluded only the arteries.
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http://dx.doi.org/10.1111/hepr.13561DOI Listing
November 2020

Transarterial- chemoembolization remains an effective therapy for intermediate-stage hepatocellular carcinoma with preserved liver function.

Hepatol Res 2020 Oct 14;50(10):1176-1185. Epub 2020 Aug 14.

Department of Radiology, IVR Center, Nara Medical University, Kashihara, Japan.

Aim: To evaluate outcomes as well as prognostic factors of transarterial chemoembolization (TACE) in intermediate-stage hepatocellular carcinoma (HCC) with preserved liver function to determine positioning of TACE.

Methods: Of 158 treatment-naïve patients with intermediate-stage HCC who received initial TACE from February 2007 to January 2016, 113 patients met the following inclusion criteria: no combined therapy within 4 weeks after initial TACE, and Child-Pugh score under 7. Response rate and overall survival were evaluated. The prognostic factors were investigated in univariate and multivariate analyses using Cox proportional hazards models. The deterioration of liver function after repeated TACE was also evaluated.

Results: The response rate was 92.7% (complete response, 63.3%; partial response, 29.4%). The median survival time was 45.2 months. Survival rates at 1, 2, and 3 years were 90.4%, 77.0%, and 60.8% respectively. Age ≥ 75 years (P = 0.022), serum α-fetoprotein level ≥ 200 ng/mL (P = .010), tumor number ≥ 11 (P = 0.008), and heterogeneous enhancement on dynamic computed tomography (P = 0.024) were poor prognostic factors. The deterioration rate of Child-Pugh score and albumin-bilirubin grade was 18.5% and 12.3%, respectively, after the first TACE, 15.6% and 5.1%, respectively, after the second TACE, and 14.5% and 11.1%, respectively, after the third TACE.

Conclusion: Superselective TACE can achieve high tumor response rates with prolonged overall survival for patients with intermediate-stage HCC with preserved liver function. Age, serum α-fetoprotein level, tumor number ≥ 11, and heterogeneous enhancement on dynamic computed tomography indicated significantly poor prognosis.
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http://dx.doi.org/10.1111/hepr.13550DOI Listing
October 2020

Home device-monitored sleep blood pressure reflects large artery stiffness: the Nagahama study.

J Hypertens 2020 12;38(12):2459-2464

Center for Gnomic Medicine, Kyoto University Graduate School of Medicine, Sakyo-ku, Kyoto.

Background: High sleep blood pressure (BP) has been suggested to be an independent risk factor for cardiovascular outcomes. To assess the applicability of sleep BP measured using a timer-equipped home device, we investigated the association between home device-measured sleep BP and large artery stiffness.

Methods: We performed a cross-sectional analysis of a dataset from the Nagahama study (N = 5916), a general population-based cohort study. Home morning BP and sleep BP were measured using a timer-equipped cuff-oscillometric device (HEM-7080IC). Office BP, carotid intima--media thickness (IMT), and brachial--ankle pulse wave velocity (baPWV) were measured at the follow-up investigation of the Nagahama study.

Results: Sleep hypertension (SBP ≥120 mmHg and/or DBP ≥70 mmHg) was associated with the arterial parameters (IMT: β = 0.051, baPWV: β = 0.141, both P < 0.001) independently of morning hypertension (IMT: β = 0.093, baPWV: β = 0.216, both P < 0.001) irrespective of antihypertensive medication status. Individuals exhibiting isolated sleep hypertension (N = 801) had thicker IMT (0.69 ± 0.14 vs. 0.64 ± 0.13 mm, P = 0.017) and faster baPWV (1,299 ± 197 vs. 1,183 ± 178 cm/s, P < 0.001) than normotensives. A sleep SBP at least 110 mmHg and a sleep DBP at least 65 mmHg were identified as the lower threshold BP values for the association with arterial parameters.

Conclusion: Sleep BP measurement using a home device may be a simple way to assess cardiovascular risks overlooked by office and home morning BP measurements.
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http://dx.doi.org/10.1097/HJH.0000000000002576DOI Listing
December 2020

Prospective associations of sleep apnea, periodic limb movements, and plasma fibrinogen level.

Sleep Breath 2021 Jun 20;25(2):617-625. Epub 2020 Jul 20.

Department of Respiratory Care and Sleep Control Medicine, Graduate School of Medicine, Kyoto University, 54 Shogoin Kawahara-cho Sakyo, Kyoto, 606-8507, Japan.

Purpose: Our previous cross-sectional study showed that periodic limb movements during sleep (PLMS) were frequently found in patients with obstructive sleep apnea (OSA) and that both OSA and PLMS were associated with higher plasma fibrinogen levels. We explored the longitudinal relationships among these factors.

Methods: Plasma fibrinogen levels were measured in 333 consecutive patients who underwent polysomnography to diagnose OSA. Patients who initiated continuous positive airway pressure (CPAP) underwent follow-up polysomnography after 3 months of CPAP use. They were categorized into groups with good or poor adherence (% days with ≥ 4 h/night of CPAP use ≥ 70% or < 70%, respectively). Changes in sleep parameters and plasma fibrinogen levels during the treatment period were compared between these groups.

Results: The cross-sectional analysis of all reviewed 333 patients indicated that fibrinogen levels were associated with the severities of OSA and PLMS. The 60 patients (27 good and 33 poor adherence) who underwent follow-up polysomnography were included in the longitudinal analysis. The median (interquartile range) periodic limb movement index did not change significantly from CPAP titration to the 3-month follow-up (good adherence: 10.5 (0-23.8) to 10.8 (0-70.2) events/h, p = 0.21; poor adherence: 1.2 (0-14.3) to 0.8 (0-15.7) events/h, p = 0.67). However, the plasma fibrinogen level significantly decreased only in the good adherence group (good adherence: baseline 275 ± 46 to follow-up 255 ± 47 mg/dl, p < 0.01; poor adherence: 277 ± 52 to 284 ± 70 mg/dl, p = 0.48).

Conclusions: These results did not support a longitudinal association between PLMS and OSA. However, good adherence to CPAP could reduce plasma fibrinogen levels, thus ameliorating elevations in plasma fibrinogen as a risk factor for future cardiovascular events.
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http://dx.doi.org/10.1007/s11325-020-02147-5DOI Listing
June 2021

Effects of platelet and phospholipids on clot formation activated by a small amount of tissue factor.

Thromb Res 2020 09 10;193:146-153. Epub 2020 Jun 10.

Department of Molecular Pathobiology and Cell Adhesion Biology, Mie University Graduate School of medicine, Tsu, Japan.

Introduction: Physiological coagulation is considered to activate coagulation factor IX (FIX) by a small amount of tissue factor (TF) and activated coagulation factor VII (FVIIa) with the presence of platelets. A Clot waveform analysis (CWA) may be useful for evaluating physiological coagulation.

Material And Methods: A CWA using a small amount of TF (CWA/sTF) was performed in platelet-rich plasma (PRP), platelet-poor plasma (PPP), several phospholipids (PLs) and patients with lupus anticoagulant (LA), idiopathic thrombocytopenic purpura (ITP) or inhibitor for FVIII.

Results: The CWA/sTF without PLs showed a shorter peak time and higher peak height in PRP than in PPP. The effect of PRP on the CWA/sTF depended on the platelet count, and PLs showed a similar effect on the CWA/sTF results in PPP. The peak time of the CWA/sTF in PRP was prolonged in patient with ITP. The CWA/sTF in PRP showed a prolonged peak time and decreased peak height of the second derivative in patient with LA. Both a shortened peak time and elevated peak height were observed in the CWA/sTF of patient with inhibitor after treatment with activated recombinant human FVII.

Conclusion: A CWA can be conducted using a small amount of TF and platelets or PL without contact activation and may be able to detect not only hemostatic abnormalities but also changes in platelet counts.
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http://dx.doi.org/10.1016/j.thromres.2020.06.018DOI Listing
September 2020

Role of serum periostin in severe obstructive sleep apnea with albuminuria: an observational study.

Respir Res 2020 Jun 9;21(1):143. Epub 2020 Jun 9.

Department of Respiratory Care and Sleep Control Medicine, Graduate School of Medicine, Kyoto University, 54 Kawaharacho, Shogoin, Sakyo-ku, Kyoto City, Kyoto prefecture, 606-8507, Japan.

Background: Periostin is a matricellular protein and is a useful marker in respiratory diseases. However, the roles of periostin in patients with obstructive sleep apnea (OSA) remain unclear. Several in vitro studies have suggested that mechanical stress, hypoxia, impaired metabolism, and kidney injury, which often accompany OSA, may upregulate the expression of periostin. Meanwhile, serum periostin level has been negatively associated with body mass index (BMI) in the general population. In this study, we hypothesized that a high level of serum periostin despite being overweight/obese may discriminate severe OSA or OSA with comorbidities from mild OSA with obesity alone. We aimed to clarify the roles of periostin in patients with OSA to assist in elucidating the heterogeneity of OSA with comorbidities.

Methods: Among patients diagnosed as OSA, we examined the associations between serum periostin levels and clinical indices, including the severity of OSA, BMI, and comorbidities, using a multifaceted approach. The serum periostin levels and clinical indices were assessed after 3 months of continuous positive airway pressure (CPAP) treatment.

Results: In 96 patients with OSA, serum periostin level was negatively correlated with BMI, albeit marginally, and tended to be higher in severe OSA than in others when adjusted for BMI. Cluster analysis identified four clusters, including two severe OSA clusters, one of which was characterized by high serum periostin levels and the presence of comorbidities, including albuminuria. In a comparative analysis of severe OSA cases (n = 53), the level of serum-free fatty acids and the frequency of albuminuria were higher in patients with high serum periostin level of ≥87 ng/mL, which was the highest quintile among all participants, than in those with low serum periostin levels (< 87 ng/mL, n = 41). In patients with severe OSA and high serum periostin levels, the levels of serum periostin and urinary albumin significantly decreased after 3 months of CPAP treatment.

Conclusions: Elevated serum periostin in patients with OSA despite being overweight/obese may be an indicator of severe OSA with comorbidities, particularly albuminuria.
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http://dx.doi.org/10.1186/s12931-020-01413-0DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7285606PMC
June 2020

Molecular Insights into the Ligand-Based Six-Proton- and Six-Electron-Transfer Processes Between Tris-ortho-Phenylenediamines and Tris-ortho-Benzoquinodiimines.

Chemistry 2020 Aug 8;26(43):9609-9619. Epub 2020 Jul 8.

Department of Applied Chemistry, Faculty of Science and Engineering, Chuo University, 1-13-27 Kasuga, Bunkyo-ku, Tokyo 112-8551, Japan.

The global demand for energy and the concerns over climate issues renders the development of alternative renewable energy sources such as hydrogen (H ) important. A high-spin (hs) Fe complex with o-phenylenediamine (opda) ligands, [Fe (opda) ] (hs-[6R] ), was reported showing photochemical H evolution. In addition, a low-spin (ls) [Fe (bqdi) ] (bqdi: o-benzoquinodiimine) (ls-[0R] ) formation by O oxidation of hs-[6R] , accompanied by ligand-based six-proton and six-electron transfer, revealed the potential of the complex with redox-active ligands as a novel multiple-proton and -electron storage material, albeit that the mechanism has not yet been understood. This paper reports that the oxidized ls-[0R][PF ] can be reduced by hydrazine giving ls-[Fe (opda)(bqdi) ][PF ] (ls-[2R][PF ] ) and ls-[Fe (opda) (bqdi)][PF ] (ls-[4R][PF ] ) with localized ligand-based proton-coupled mixed-valence (LPMV) states. The first isolation and characterization of the key intermediates with LPMV states offer unprecedented molecular insights into the design of photoresponsive molecule-based hydrogen-storage materials.
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http://dx.doi.org/10.1002/chem.202001873DOI Listing
August 2020
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