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1.
Elife. 2019 Jun 24;8. pii: e48054. doi: 10.7554/eLife.48054. [Epub ahead of print]

An elusive electron shuttle from a facultative anaerobe.

Author information

1
Department of Biological Chemistry and Molecular Pharmacology, Harvard Medical School, Boston, United States.
2
Molecular Foundry Division, Lawrence Berkeley National Laboratory, University of California, Berkeley, Berkeley, United States.

Abstract

Some anaerobic bacteria use insoluble minerals as terminal electron acceptors and discovering the ways in which electrons move through the membrane barrier to the exterior acceptor forms an active field of research with implications for both bacterial physiology and bioenergy. A previous study suggested that Shewanella oneidensis MR-1 utilizes a small, polar, redox active molecule that serves as an electron shuttle between the bacteria and insoluble acceptors, but the shuttle itself has never been identified. Through isolation and synthesis, we identify it as ACNQ (2-amino-3-carboxy-1,4-naphthoquinone), a soluble analog of menaquinone. ACNQ is derived from DHNA (1,4-dihydroxy-2-naphthoic acid) in a non-enzymatic process that frustrated genetic approaches to identify the shuttle. Both ACNQ and DHNA restore reduction of AQDS under anaerobic growth in menaquinone-deficient mutants. Bioelectrochemistry analyses reveal that ACNQ (-0.32 VAg/AgCl) contributes to the extracellular electron transfer (EET) as an electron shuttle, without altering menaquinone generation or EET related cytochrome c expression.

KEYWORDS:

biochemistry; chemical biology; infectious disease; microbiology; none

2.
Inflamm Res. 2019 Jun 21. doi: 10.1007/s00011-019-01262-8. [Epub ahead of print]

Macrophage lipid accumulation in the presence of immunosuppressive drugs mycophenolate mofetil and cyclosporin A.

Author information

1
Department of Medicine and Winthrop Research Institute, NYU Long Island School of Medicine, NYU Winthrop Hospital, 101 Mineola Boulevard, Suite 4-004, Mineola, NY, 11501, USA.
2
Department of Medicine and Winthrop Research Institute, NYU Long Island School of Medicine, NYU Winthrop Hospital, 101 Mineola Boulevard, Suite 4-004, Mineola, NY, 11501, USA. Allison.Reiss@nyulangone.org.

Abstract

OBJECTIVE:

Mycophenolate (MPA) and cyclosporin A (CsA) are two immunosuppressive agents currently used for the treatment of autoimmune diseases. However, reports regarding their effects on inflammation and lipid handling are controversial. Here, we compare the effect of these two drugs on the expression of proteins involved in cholesterol handling and lipid accumulation in a macrophage cell system utilizing M0, M1 and M2 human macrophages and in murine bone marrow-derived macrophages (BMDM).

METHODS:

Differentiated M0, M1 and M2 subsets of THP-1 human macrophages were subjected to various concentrations of either MPA or CsA. Expression of proteins involved in reverse cholesterol transport (ABCA1 and 27-hydroxylase) and scavenger receptors, responsible for uptake of modified lipids (CD36, ScR-A1, CXCL16 and LOX-1), were evaluated by real-time PCR and confirmed with Western blot. DiI-oxidized LDL internalization assay was used to assess foam cell formation. The influence of MPA was also evaluated in BMDM obtained from atherosclerosis-prone transgenic mice, ApoE-/- and ApoE-/-Fas-/-.

RESULTS:

In M0 macrophages, MPA increased expression of ABCA1 and CXCL16 in a concentration-dependent manner. In M1 THP-1 macrophages, MPA caused a significant increase of 27-hydroxylase mRNA and CD36 and SR-A1 receptor mRNAs. Exposure of M2 macrophages to MPA also stimulated expression of 27-hydroxylase, while downregulating all evaluated scavenger receptors. In contrast, CsA had no impact on cholesterol efflux in M0 and M1 macrophages, but significantly augmented expression of ABCA1 and 27-hydroxylase in M2 macrophages. CsA significantly increased expression of the LOX1 receptor in naïve macrophages, downregulated expression of CD36 and SR-A1 in the M1 subpopulation and upregulated expression of all evaluated scavenger receptors. However, CsA enhanced foam cell transformation in M0 and M2 macrophages, while MPA had no effect on foam cell formation unless used at a high concentration in the M2 subtype.

CONCLUSIONS:

Our results clearly underline the importance of further evaluation of the effects of these drugs when used in atherosclerosis-prone patients with autoimmune or renal disease.

KEYWORDS:

Autoimmune disease; CVD; Foam cell formation; Immunosuppressive agent; M1 and M2 subtypes of macrophages; Reverse cholesterol transport; Scavenger receptors

3.
Macromol Biosci. 2019 Jun 21:e1900130. doi: 10.1002/mabi.201900130. [Epub ahead of print]

Scaffolds for Sustained Release of Ambroxol Hydrochloride, a Pharmacological Chaperone That Increases the Activity of Misfolded β-Glucocerebrosidase.

Author information

1
Departament d'Enginyeria Química and Barcelona Research Center for Multiscale Science and Engineering, EEBE, Universitat Politècnica de Catalunya, C/Eduard Maristany, 10-14, 08019, Barcelona, Spain.
2
Centre for Genomic Regulation (CRG), The Barcelona Institute of Science and Technology, 08003, Barcelona, Spain.
3
Universitat Pompeu Fabra (UPF), 08002, Barcelona, Spain.
4
Institute for Bioengineering of Catalonia (IBEC), The Barcelona Institute of Science and Technology, Baldiri Reixac 10-12, 08028, Barcelona, Spain.

Abstract

Ambroxol is a pharmacological chaperone (PC) for Gaucher disease that increases lysosomal activity of misfolded β-glucocerebrosidase (GCase) while displaying a safe toxicological profile. In this work, different poly(ε-caprolactone) (PCL)-based systems are developed to regulate the sustained release of small polar drugs in physiological environments. For this purpose, ambroxol is selected as test case since the encapsulation and release of PCs using polymeric scaffolds have not been explored yet. More specifically, ambroxol is successfully loaded in electrospun PCL microfibers, which are subsequently coated with additional PCL layers using dip-coating or spin-coating. The time needed to achieve 80% release of loaded ambroxol increases from ≈15 min for uncoated fibrous scaffolds to 3 days and 1 week for dip-coated and spin-coated systems, respectively. Furthermore, it is proven that the released drug maintains its bioactivity, protecting GCase against induced thermal denaturation.

KEYWORDS:

Gaucher's disease; electrospinning; lysosomal storage disorders; misfolding diseases; poly(ε-caprolactone); polyester; release regulation

4.
Adv Mater. 2019 Jun 21:e1901745. doi: 10.1002/adma.201901745. [Epub ahead of print]

Nanostructured Back Reflectors for Efficient Colloidal Quantum-Dot Infrared Optoelectronics.

Author information

1
Department of Electrical and Computer Engineering, University of Toronto, 10 King's College Road, Toronto, Ontario, M5S 3G4, Canada.
2
Institut de Ciència de Materials de Barcelona (ICMAB-CSIC), Campus de la UAB, 08193, Bellaterra, Catalonia, Spain.

Abstract

Colloidal quantum dots (CQDs) can be used to extend the response of solar cells, enabling the utilization of solar power that lies to the red of the bandgap of c-Si and perovskites. To achieve largely complete absorption of infrared (IR) photons in CQD solids requires thicknesses on the micrometer range; however, this exceeds the typical diffusion lengths (≈300 nm) of photoexcited charges in these materials. Nanostructured metal back electrodes that grant the cell efficient IR light trapping in thin active layers with no deterioration of the electrical properties are demonstrated. Specifically, a new hole-transport layer (HTL) is developed and directly nanostructured. Firstly, a material set to replace conventional rigid HTLs in CQD devices is developed with a moldable HTL that combines the mechanical and chemical requisites for nanoimprint lithography with the optoelectronic properties necessary to retain efficient charge extraction through an optically thick layer. The new HTL is nanostructured in a 2D lattice and conformally coated with MoO3 /Ag. The photonic structure in the back electrode provides a record photoelectric conversion efficiency of 86%, beyond the Si bandgap, and a 22% higher IR power conversion efficiency compared to the best previous reports.

KEYWORDS:

colloidal quantum dots; conjugated polymers; hole transporting layers; infrared optoelectronics; nanoimprinting

5.
Sleep Breath. 2019 Jun 21. doi: 10.1007/s11325-019-01874-8. [Epub ahead of print]

Electrocardiogram-based sleep analysis for sleep apnea screening and diagnosis.

Author information

1
Center for Dynamical Biomarkers, Division of Interdisciplinary Medicine and Biotechnology, Beth Israel Deaconess Medical Center, Harvard Medical School, 330 Brookline Avenue, Boston, MA, 02215, USA. dr.yan.ma@gmail.com.
2
Department of Otolaryngology and South Campus Sleep Center, Guang'anmen Hospital, China Academy of Chinese Medical Sciences, Beijing, 100053, China. sunsc0922@163.com.
3
Nanjing Integrated Traditional Chinese and Western Medicine Hospital, Nanjing, 210000, China.
4
Center for Dynamical Biomarkers, Division of Interdisciplinary Medicine and Biotechnology, Beth Israel Deaconess Medical Center, Harvard Medical School, 330 Brookline Avenue, Boston, MA, 02215, USA.
5
China-Japan Friendship Hospital, Beijing, 100029, China.

Abstract

PURPOSE:

Despite the increasing number of research studies of cardiopulmonary coupling (CPC) analysis, an electrocardiogram-based technique, the use of CPC in underserved population remains underexplored. This study aimed to first evaluate the reliability of CPC analysis for the detection of obstructive sleep apnea (OSA) by comparing with polysomnography (PSG)-derived sleep outcomes.

METHODS:

Two hundred five PSG data (149 males, age 46.8 ± 12.8 years) were used for the evaluation of CPC regarding the detection of OSA. Automated CPC analyses were based on ECG signals only. Respiratory event index (REI) derived from CPC and apnea-hypopnea index (AHI) derived from PSG were compared for agreement tests.

RESULTS:

CPC-REI positively correlated with PSG-AHI (r = 0.851, p < 0.001). After adjusting for age and gender, CPC-REI and PSG-AHI were still significantly correlated (r = 0.840, p < 0.001). The overall results of sensitivity and specificity of CPC-REI were good.

CONCLUSION:

Compared with the gold standard PSG, CPC approach yielded acceptable results among OSA patients. ECG recording can be used for the screening or diagnosis of OSA in the general population.

KEYWORDS:

Autonomic nervous system; Cardiopulmonary coupling; Electrocardiogram; Obstructive sleep apnea; Polysomnography; Portable monitoring

6.
Sci Rep. 2019 Jun 20;9(1):8876. doi: 10.1038/s41598-019-45184-1.

Genome-wide alternative splicing landscapes modulated by biotrophic sugarcane smut pathogen.

Author information

1
Texas A&M AgriLife Research & Extension Center, Texas A&M University, Weslaco, TX, USA.
2
Departamento de Genética, Universidade de São Paulo, Escola Superior de Agricultura "Luiz de Queiroz," Piracicaba, São Paulo, Brazil.
3
Universidade Tecnológica Federal do Paraná, Toledo, Paraná, Brazil.
4
Department of Soil & Crop Sciences, Texas A&M University, College Station, TX, USA.
5
Texas A&M AgriLife Research & Extension Center, Texas A&M University, Weslaco, TX, USA. kkmandadi@tamu.edu.
6
Department of Plant Pathology & Microbiology, Texas A&M University, College Station, TX, USA. kkmandadi@tamu.edu.

Abstract

Alternative splicing (AS) promotes transcriptome and proteome diversity during growth, development, and stress responses in eukaryotes. Genome-wide studies of AS in sugarcane (Saccharum spp.) are lacking, mainly due to the absence of a high-quality sequenced reference genome, sugarcane's large, complex genome, and the variable chromosome numbers and polyploidy of sugarcane cultivars. Here, we analyzed changes in the sugarcane isoform-level transcriptome and AS landscape during infection with the smut fungus (Sporisorium scitamineum) using a hybrid approach involving Sorghum bicolor reference-based and Trinity de novo mapping tools. In total, this analysis detected 16,039 and 15,379 transcripts (≥2 FPKM) at 5 and 200 days after infection, respectively. A conservative estimate of isoform-level expression suggested that approximately 5,000 (14%) sugarcane genes undergo AS. Differential expression analysis of the alternatively spliced genes in healthy and smut-infected sugarcane revealed 896 AS events modulated at different stages of infection. Gene family and gene ontology functional enrichment analysis of the differentially spliced genes revealed overrepresentation of functional categories related to the cell wall, defense, and redox homeostasis pathways. Our study provides novel insight into the AS landscape of sugarcane during smut disease interactions.

PMID:
31222001
DOI:
10.1038/s41598-019-45184-1
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7.
J Bone Miner Res. 2019 Jun 20. doi: 10.1002/jbmr.3727. [Epub ahead of print]

Pentosidine Is Associated With Cortical Bone Geometry and Insulin Resistance in Otherwise Healthy Children.

Author information

1
Department of Foods and Nutrition, The University of Georgia, Athens, GA, USA.
2
Department of Chemistry, University of Rhode Island, Kingston, RI, USA.

Abstract

Pentosidine is an advanced glycation end product (AGE) associated with fracture in adults with diabetes. AGE accumulation in bone collagen contributes to bone fragility but might also adversely influence bone turnover and, consequently, bone geometry. The relationships between AGEs and bone health have yet to be studied in children. Thus, the objective of this study was to assess relationships between pentosidine and cortical bone volumetric density, geometry, and estimated strength in children. Participants were otherwise healthy black and white boys and girls, ages 9 to 13 years, who were at sexual maturation stage 2 or 3 (N = 160). Tibia and radius cortical bone and muscle area (66% site) were assessed via pQCT. In fasting sera, insulin, glucose, and pentosidine were measured. The Quantitative Insulin Sensitivity Check Index (QUICKI), a measure of insulin sensitivity, was calculated. While controlling for race, sex, maturation, and height, pentosidine negatively correlated with QUICKI (P < 0.05). In unadjusted analyses, pentosidine was associated with lower radius and tibia cortical volumetric bone mineral density, bone mineral content (Ct.BMC), area (Ct.Ar), and thickness (Ct.Th); a larger radius endosteal circumference (Endo.Circ); and lower tibia polar strength strain index (all P < 0.05). While controlling for race, sex, maturation, height, and muscle area, pentosidine was negatively associated with tibia Ct.BMC, Ct.Ar, and Ct.Th but positively associated with Endo.Circ (all P < 0.05). Linear regression revealed a significant interaction between pentosidine and QUICKI in relation to tibia Ct.Th (pinteraction = 0.049), indicating that the negative relationship between pentosidine and Ct.Th was stronger in those with lower QUICKI (ie, greater insulin resistance). This is the first study to report evidence of a potentially adverse influence of AGEs on bone strength in otherwise healthy children. This relationship was strongest in children with the greatest insulin resistance, supporting further work in youth with chronic metabolic health conditions.

KEYWORDS:

ADVANCED GLYCATION END PRODUCT; BONE GEOMETRY IN CHILDREN; INSULIN RESISTANCE; PENTOSIDINE

PMID:
31220375
DOI:
10.1002/jbmr.3727
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8.
Sci Rep. 2019 Jun 19;9(1):8801. doi: 10.1038/s41598-019-45238-4.

Evaluation of Neurosecretome from Mesenchymal Stem Cells Encapsulated in Silk Fibroin Hydrogels.

Author information

1
Center for Biomedical Technology, Universidad Politécnica de Madrid, Madrid, Spain.
2
Neurocomputing and Neurorobotics Research Group: Faculty of Biology and Faculty of Optics, Universidad Complutense de Madrid., Madrid, Spain.
3
Brain Plasticity Group. Health Research Institute of the Hospital Clínico San Carlos (IdISSC), Madrid, Spain.
4
GReD, UMR CNRS 6293 - INSERM U1103 - Université Clermont Auvergne, Faculté de Medicine, Clermont-Ferrand, France.
5
Departamento de Ciencia de Materiales. ETSI Caminos, Canales y Puertos, Universidad Politécnica de Madrid, Madrid, Spain.
6
Biomedical Research Networking Center in Bioengineering Biomaterials and Nanomedicine (CIBER-BBN), Madrid, Spain.
7
Departamento de Tecnología Fotónica y Bioingeniería. ETSI Telecomunicaciones, Universidad Politécnica de Madrid, Madrid, Spain.
8
Center for Biomedical Technology, Universidad Politécnica de Madrid, Madrid, Spain. daniel.gonzalez@ctb.upm.es.
9
Departamento de Tecnología Fotónica y Bioingeniería. ETSI Telecomunicaciones, Universidad Politécnica de Madrid, Madrid, Spain. daniel.gonzalez@ctb.upm.es.
10
Biomedical Research Networking Center in Bioengineering Biomaterials and Nanomedicine (CIBER-BBN), Madrid, Spain. daniel.gonzalez@ctb.upm.es.

Abstract

Physical and cognitive disabilities are hallmarks of a variety of neurological diseases. Stem cell-based therapies are promising solutions to neuroprotect and repair the injured brain and overcome the limited capacity of the central nervous system to recover from damage. It is widely accepted that most benefits of different exogenously transplanted stem cells rely on the secretion of different factors and biomolecules that modulate inflammation, cell death and repair processes in the damaged host tissue. However, few cells survive in cerebral tissue after transplantation, diminishing the therapeutic efficacy. As general rule, cell encapsulation in natural and artificial polymers increases the in vivo engraftment of the transplanted cells. However, we have ignored the consequences of such encapsulation on the secretory activity of these cells. In this study, we investigated the biological compatibility between silk fibroin hydrogels and stem cells of mesenchymal origin, a cell population that has gained increasing attention and popularity in regenerative medicine. Although the survival of mesenchymal stem cells was not affected inside hydrogels, this biomaterial format caused adhesion and proliferation deficits and impaired secretion of several angiogenic, chemoattractant and neurogenic factors while concurrently potentiating the anti-inflammatory capacity of this cell population through a massive release of TGF-Beta-1. Our results set a milestone for the exploration of engineering polymers to modulate the secretory activity of stem cell-based therapies for neurological disorders.

PMID:
31217546
DOI:
10.1038/s41598-019-45238-4
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9.
Sci Rep. 2019 Jun 19;9(1):8742. doi: 10.1038/s41598-019-45009-1.

Environmental microcystin targets the microbiome and increases the risk of intestinal inflammatory pathology via NOX2 in underlying murine model of Nonalcoholic Fatty Liver Disease.

Author information

1
Environmental Health and Disease Laboratory, Department of Environmental Health Sciences, University of South Carolina, Columbia, USA.
2
NIEHS Center for Oceans and Human Health on Climate Change Interactions, Department of Environmental Health Sciences, University of South Carolina, Columbia, USA.
3
Pathology, Microbiology and Immunology, University of South Carolina School of Medicine, Columbia, USA.
4
Department of Environmental Science, Baylor University, Waco, USA.
5
Environmental Health and Disease Laboratory, Department of Environmental Health Sciences, University of South Carolina, Columbia, USA. schatt@mailbox.sc.edu.
6
NIEHS Center for Oceans and Human Health on Climate Change Interactions, Department of Environmental Health Sciences, University of South Carolina, Columbia, USA. schatt@mailbox.sc.edu.

Abstract

With increased climate change pressures likely to influence harmful algal blooms, exposure to microcystin, a known hepatotoxin and a byproduct of cyanobacterial blooms can be a risk factor for NAFLD associated comorbidities. Using both in vivo and in vitro experiments we show that microcystin exposure in NAFLD mice cause rapid alteration of gut microbiome, rise in bacterial genus known for mediating gut inflammation and lactate production. Changes in the microbiome were strongly associated with inflammatory pathology in the intestine, gut leaching, tight junction protein alterations and increased oxidative tyrosyl radicals. Increased lactate producing bacteria from the altered microbiome was associated with increased NOX-2, an NADPH oxidase isoform. Activationof NOX2 caused inflammasome activation as shown by NLRP3/ASCII and NLRP3/Casp-1 colocalizations in these cells while use of mice lacking a crucial NOX2 component attenuated inflammatory pathology and redox changes. Mechanistically, NOX2 mediated peroxynitrite species were primary to inflammasome activation and release of inflammatory mediators. Thus, in conclusion, microcystin exposure in NAFLD could significantly alter intestinal pathology especially by the effects on microbiome and resultant redox status thus advancing our understanding of the co-existence of NAFLD-linked inflammatory bowel disease phenotypes in the clinic.

PMID:
31217465
DOI:
10.1038/s41598-019-45009-1
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10.
Polymers (Basel). 2019 Jun 18;11(6). pii: E1057. doi: 10.3390/polym11061057.

Thermally Healable and Recyclable Graphene-Nanoplate/Epoxy Composites Via an In-Situ Diels-Alder Reaction on the Graphene-Nanoplate Surface.

Author information

1
Division of Semiconductor and Chemical Engineering, Chonbuk National University, Baekjedaero 567, Jeonju 54896, Korea. ohcho38@naver.com.
2
Division of Semiconductor and Chemical Engineering, Chonbuk National University, Baekjedaero 567, Jeonju 54896, Korea. ldi4084@naver.com.
3
R & D Center, Lotte Advanced Materials, Sandan-ro 334-27, Yeosu 59616, Korea. jh711.park@lottechem.com.
4
Division of Semiconductor and Chemical Engineering, Chonbuk National University, Baekjedaero 567, Jeonju 54896, Korea. daisoolee@jbnu.ac.kr.

Abstract

In this work, thermally healable graphene-nanoplate/epoxy (GNP/EP) nanocomposites were investigated. GNPs were used as reinforcement and crosslinking platforms for the diglycidyl ether of bisphenol A-based epoxy resin (DGEBA) through the Diels-Alder (DA) reaction with furfurylamine (FA). The GNPs and FA could then be used as a derivative of diene and dienophile in the DA reaction. It was expected that the combination of GNPs and FA in DGEBA would produce composites based on the interfacial properties of the components. We confirmed the DA reaction of GNPs and FA at the interface during curing of the GNP/EP nanocomposites. This procedure is simple and solvent-free. DA and retro DA reactions of the obtained composites were demonstrated, and the thermal healing properties were evaluated. The behavior of the GNP/EP nanocomposites in the DA reaction is similar to that of thermosetting polymers at low temperatures due to crosslinking by the DA reaction, and the nanocomposites can be recycled by a retro DA reaction at high temperatures.

KEYWORDS:

Diels-Alder reaction; epoxy composites; graphene-nanoplate; thermally healing

PMID:
31216683
DOI:
10.3390/polym11061057
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11.
Molecules. 2019 Jun 18;24(12). pii: E2262. doi: 10.3390/molecules24122262.

Investigation of the Binding Affinity of a Broad Array of l-Fucosides with Six Fucose-Specific Lectins of Bacterial and Fungal Origin.

Author information

1
Department of Pharmaceutical Chemistry, University of Debrecen, Egyetem tér 1, H-4032 Debrecen, Hungary. le.thai.son@pharm.unideb.hu.
2
Central European Institute of Technology, Masaryk University, Kamenice 5, 625 00 Brno, Czech Republic. malinovska@mail.muni.cz.
3
National Centre for Biomolecular Research, Faculty of Science, Masaryk University, Kotlářská 2, 611 37 Brno, Czech Republic. malinovska@mail.muni.cz.
4
Department of Biochemistry, Faculty of Science, Charles University, Albertov 2030, 128 40 Prague 2, Czech Republic. michael.vaskova@gmail.com.
5
Department of Pharmaceutical Chemistry, University of Debrecen, Egyetem tér 1, H-4032 Debrecen, Hungary. mezo.erika@science.unideb.hu.
6
Department of Pharmaceutical Chemistry, University of Debrecen, Egyetem tér 1, H-4032 Debrecen, Hungary. kelemen.viktor@pharm.unideb.hu.
7
Department of Pharmaceutical Chemistry, University of Debrecen, Egyetem tér 1, H-4032 Debrecen, Hungary. borbas.aniko@pharm.unideb.hu.
8
Department of Biochemistry, Faculty of Science, Charles University, Albertov 2030, 128 40 Prague 2, Czech Republic. petr.hodek@natur.cuni.cz.
9
Central European Institute of Technology, Masaryk University, Kamenice 5, 625 00 Brno, Czech Republic. michaw@chemi.muni.cz.
10
National Centre for Biomolecular Research, Faculty of Science, Masaryk University, Kotlářská 2, 611 37 Brno, Czech Republic. michaw@chemi.muni.cz.
11
Department of Biochemistry, Faculty of Science, Masaryk University, Kotlářská 2, 611 37 Brno, Czech Republic. michaw@chemi.muni.cz.
12
Department of Pharmaceutical Chemistry, University of Debrecen, Egyetem tér 1, H-4032 Debrecen, Hungary. michaela.wimmerova@ceitec.muni.cz.

Abstract

Series of multivalent α-l-fucoside containing glycoclusters and variously decorated l-fucosides were synthesized to find potential inhibitors of fucose-specific lectins and study the structure-binding affinity relationships. Tri- and tetravalent fucoclusters were built using copper-mediated azide-alkyne click chemistry. Series of fucoside monomers and dimers were synthesized using various methods, namely glycosylation, an azide-alkyne click reaction, photoinduced thiol-en addition, and sulfation. The interactions between compounds with six fucolectins of bacterial or fungal origin were tested using a hemagglutination inhibition assay. As a result, a tetravalent, α-l-fucose presenting glycocluster showed to be a ligand that was orders of magnitude better than a simple monosaccharide for tested lectins in most cases, which can nominate it as a universal ligand for studied lectins. This compound was also able to inhibit the adhesion of Pseudomonas aeruginosa cells to human epithelial bronchial cells. A trivalent fucocluster with a protected amine functional group also seems to be a promising candidate for designing glycoconjugates and chimeras.

KEYWORDS:

cystic fibrosis; glycoclusters; hemagglutination; l-fucosides; lectins; multivalency

PMID:
31216664
DOI:
10.3390/molecules24122262
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12.
Materials (Basel). 2019 Jun 18;12(12). pii: E1957. doi: 10.3390/ma12121957.

Design, Synthesis, Structure and Properties of Ba-Doped Derivatives of SrCo0.95Ru0.05O3-δ Perovskite as Cathode Materials for SOFCs.

Author information

1
Instituto de Ciencia de Materiales de Madrid, C.S.I.C., Cantoblanco, E-28049 Madrid, Spain. sabisha.es@gmail.com.
2
Instituto de Ciencia de Materiales de Madrid, C.S.I.C., Cantoblanco, E-28049 Madrid, Spain. vcascos@icmm.csic.es.
3
Instituto de Ciencia de Materiales de Madrid, C.S.I.C., Cantoblanco, E-28049 Madrid, Spain. loreto.troncoso@uach.cl.
4
Instituto de Materiales y Procesos Termomecánicos, Universidad Austral de Chile, General Lagos, 2086, 5111187 Valdivia, Chile. loreto.troncoso@uach.cl.
5
INQUIMAE, Departamento de Química Inorgánica, Analítica y Química Física, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Buenos Aires C1428EGA, Argentina. alarralde@qi.fcen.uba.ar.
6
Institut Laue Langevin, BP 156X, F-38042 Grenoble, France. ferndiaz@ill.eu.
7
Instituto de Ciencia de Materiales de Madrid, C.S.I.C., Cantoblanco, E-28049 Madrid, Spain. ja.alonso@icmm.csic.es.

Abstract

We have designed and prepared a novel cathode material for solid oxide fuel cell (SOFC) based on SrCo0.95Ru0.05O3-δ perovskite. We have partially replaced Sr by Ba in Sr0.9Ba0.1Co0.95Ru0.05O3-δ (SBCRO) in order to expand the unit-cell size, thereby improving the ionic diffusion of O2- through the crystal lattice. The characterization of this new oxide has been studied at room temperature by X-ray diffraction (XRD) and neutron powder diffraction (NPD) experiments. At room temperature, SBCRO perovskite crystallizes in the P4/mmm tetragonal space group, as observed from NDP data. The maximum conductivity value of 18.6 S cm-1 is observed at 850 °C. Polarization resistance measurements on LSGM electrolyte demonstrate an improvement in conductivity with respect to the parent Sr-only perovskite cathode. A good chemical compatibility and an adequate thermal expansion coefficient make this oxide auspicious for using it as a cathode in SOFC.

KEYWORDS:

IT-SOFC; SrCoO3; cathode; neutron diffraction; perovskite

PMID:
31216661
DOI:
10.3390/ma12121957
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13.
Int J Mol Sci. 2019 Jun 18;20(12). pii: E2962. doi: 10.3390/ijms20122962.

Analysis of the TP53 Deleterious Single Nucleotide Polymorphisms Impact on Estrogen Receptor Alpha-p53 Interaction: A Machine Learning Approach.

Author information

1
Department of Zoology, Sri Venkateswara University, Tirupati 517502, India. cksnaidu@gmail.com.
2
Department of Pathology, Microbiology and Immunology, University of South Carolina School of Medicine, Columbia, SC 29208, USA. cksnaidu@gmail.com.
3
Department of Pathology, Microbiology and Immunology, University of South Carolina School of Medicine, Columbia, SC 29208, USA. Mitzi.Nagarkatti@uscmed.sc.edu.
4
Department of Pathology, Microbiology and Immunology, University of South Carolina School of Medicine, Columbia, SC 29208, USA. prakash@mailbox.sc.edu.
5
Department of Zoology, Sri Venkateswara University, Tirupati 517502, India. ysuneethareddy4@gmail.com.

Abstract

Breast cancer is a leading cancer type and one of the major health issues faced by women around the world. Some of its major risk factors include body mass index, hormone replacement therapy, family history and germline mutations. Of these risk factors, estrogen levels play a crucial role. Among the estrogen receptors, estrogen receptor alpha (ERα) is known to interact with tumor suppressor protein p53 directly thereby repressing its function. Previously, we have studied the impact of deleterious breast cancer-associated non-synonymous single nucleotide polymorphisms (nsnps) rs11540654 (R110P), rs17849781 (P278A) and rs28934874 (P151T) in TP53 gene on the p53 DNA-binding core domain. In the present study, we aimed to analyze the impact of these mutations on p53-ERα interaction. To this end, we, have modelled the full-length structure of human p53 and validated its quality using PROCHECK and subjected it to energy minimization using NOMAD-Ref web server. Three-dimensional structure of ERα activation function-2 (AF-2) domain was downloaded from the protein data bank. Interactions between the modelled native and mutant (R110P, P278A, P151T) p53 with ERα was studied using ZDOCK. Machine learning predictions on the interactions were performed using Weka software. Results from the protein-protein docking showed that the atoms, residues and solvent accessibility surface area (SASA) at the interface was increased in both p53 and ERα for R110P mutation compared to the native complexes indicating that the mutation R110P has more impact on the p53-ERα interaction compared to the other two mutants. Mutations P151T and P278A, on the other hand, showed a large deviation from the native p53-ERα complex in atoms and residues at the surface. Further, results from artificial neural network analysis showed that these structural features are important for predicting the impact of these three mutations on p53-ERα interaction. Overall, these three mutations showed a large deviation in total SASA in both p53 and ERα. In conclusion, results from our study will be crucial in making the decisions for hormone-based therapies against breast cancer.

KEYWORDS:

ERα; TP53; breast cancer; genetic factors; machine learning; single nucleotide polymorphism

PMID:
31216622
DOI:
10.3390/ijms20122962
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14.
J Cell Mol Med. 2019 Jun 19. doi: 10.1111/jcmm.14383. [Epub ahead of print]

Metabolic signature associated with parameters of the complete blood count in apparently healthy individuals.

Author information

1
Institute of Clinical Chemistry and Laboratory Medicine, University Medicine Greifswald, Greifswald, Germany.
2
German Centre for Cardiovascular Disease (DZHK e.V.), partner site Greifswald, Greifswald, Germany.
3
Institute of Bioinformatics and Systems Biology, Helmholtz Zentrum München, Neuherberg, Germany.
4
Institute of Experimental Genetics, Genome Analysis Centre, Helmholtz Zentrum München, Neuherberg, Germany.
5
Lehrstuhl für Experimentelle Genetik, Technische Universität München, Freising-Weihenstephan, Germany.
6
DZD (German Centre for Diabetes Research), München-Neuherberg, Germany.
7
Institute for Community Medicine, University Medicine Greifswald, Greifswald, Germany.
8
DZD (German Centre for Diabetes Research), site Greifswald, Greifswald, Germany.

Abstract

Metabolomics studies now approach large sample sizes and the health characterization of the study population often include complete blood count (CBC) results. Upon careful interpretation the CBC aids diagnosis and provides insight into the health status of the patient within a clinical setting. Uncovering metabolic signatures associated with parameters of the CBC in apparently healthy individuals may facilitate interpretation of metabolomics studies in general and related to diseases. For this purpose 879 subjects from the population-based Study of Health in Pomerania (SHIP)-TREND were included. Using metabolomics data resulting from mass-spectrometry based measurements in plasma samples associations of specific CBC parameters with metabolites were determined by linear regression models. In total, 118 metabolites significantly associated with at least one of the CBC parameters. Strongest associations were observed with metabolites of heme degradation and energy production/consumption. Inverse association seen with mean corpuscular volume and mean corpuscular haemoglobin comprised metabolites potentially related to kidney function. The presently identified metabolic signatures are likely derived from the general function and formation/elimination of blood cells. The wealth of associated metabolites strongly argues to consider CBC in the interpretation of metabolomics studies, in particular if mutual effects on those parameters by the disease of interest are known.

KEYWORDS:

apparently healthy; blood cell metabolism; complete blood count; metabolomics; population-based study

PMID:
31215770
DOI:
10.1111/jcmm.14383
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15.
Materials (Basel). 2019 Jun 17;12(12). pii: E1953. doi: 10.3390/ma12121953.

Expandable Layered Hybrid Materials Based on Individual 1D Metalorganic Nanoribbons.

Author information

1
Instituto de Tecnología Química, Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas, Avenida de los Naranjos s/n, E-46022 Valencia, Spain. josemmorenorodriguez@gmail.com.
2
Instituto de Tecnología Química, Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas, Avenida de los Naranjos s/n, E-46022 Valencia, Spain. avelty@itq.upv.es.
3
Instituto de Tecnología Química, Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas, Avenida de los Naranjos s/n, E-46022 Valencia, Spain. udiaz@itq.upv.es.

Abstract

Different metalorganic lamellar hybrid materials based on associated nanoribbons were synthesized by the use of alkyl-benzyl monocarboxylate spacers, containing alkyl tails with variable lengths, which acted like structural growing inhibitors. These molecular agents were perpendicularly located and coordinated to aluminium nodes in the interlayer space, controlling the separation between individual structure sub-units. The hybrid materials were studied by X-ray diffraction (XRD), chemical and thermogravimetrical analysis (TGA), nuclear magnetic resonance (NMR) and infrared spectroscopy (IR), and field emission scanning electron microscopy (FESEM)/transmission electron microscopy (TEM), showing their physicochemical properties. The specific capacity of the metalorganic materials to be exfoliated through post-synthesis treatments, using several solvents due to the presence of 1D structure sub-units and a marked hydrophobic nature, was also evidenced.

KEYWORDS:

MOFs; exfoliation; growing inhibitors; hybrids; layered materials; monocarboxylate spacers

PMID:
31213003
DOI:
10.3390/ma12121953
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16.
Cancers (Basel). 2019 Jun 17;11(6). pii: E835. doi: 10.3390/cancers11060835.

Determination of PD-L1 Expression in Circulating Tumor Cells of NSCLC Patients and Correlation with Response to PD-1/PD-L1 Inhibitors.

Author information

1
Department of Oncology, Hematology and Bone Marrow Transplantation with section Pneumology, Hubertus Wald University Comprehensive Cancer Center Hamburg, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. m.janning@uke.de.
2
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. m.janning@uke.de.
3
Department of Oncology, Hematology and Bone Marrow Transplantation with section Pneumology, Hubertus Wald University Comprehensive Cancer Center Hamburg, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. francakobus@yahoo.de.
4
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. francakobus@yahoo.de.
5
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. a.babayan@uke.de.
6
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. h.wikman@uke.de.
7
Department of Oncology, Hematology and Bone Marrow Transplantation with section Pneumology, Hubertus Wald University Comprehensive Cancer Center Hamburg, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. j.velthaus@uke.de.
8
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. j.velthaus@uke.de.
9
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. so.bergmann@uke.de.
10
Institute of Hematopathology Hamburg HpH, 22547 Hamburg, Germany. schatz@hp-hamburg.de.
11
Institute of Hematopathology Hamburg HpH, 22547 Hamburg, Germany. falk@hp-hamburg.de.
12
Department of Oncology, Hematology and Bone Marrow Transplantation with section Pneumology, Hubertus Wald University Comprehensive Cancer Center Hamburg, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. LarsArne.Berger@hopa.de.
13
Department of Oncology, Hematology and Bone Marrow Transplantation with section Pneumology, Hubertus Wald University Comprehensive Cancer Center Hamburg, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. lisamarie.boettcher@googlemail.com.
14
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. lisamarie.boettcher@googlemail.com.
15
Department of Oncology, Hematology and Bone Marrow Transplantation with section Pneumology, Hubertus Wald University Comprehensive Cancer Center Hamburg, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. s.paesler@uke.de.
16
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. s.paesler@uke.de.
17
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. tobias.gorges@astrazeneca.com.
18
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. linda.scarrott@boehringer-ingelheim.com.
19
Boehringer Ingelheim Pharma GmbH & Co. KG, 88397 Biberach, Germany. linda.scarrott@boehringer-ingelheim.com.
20
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. c.hille@uke.de.
21
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. s.joosse@uke.de.
22
Institute of Pathology, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. r.simon@uke.de.
23
Institute of Hematopathology Hamburg HpH, 22547 Hamburg, Germany. mtiemann@hp-hamburg.de.
24
Department of Oncology, Hematology and Bone Marrow Transplantation with section Pneumology, Hubertus Wald University Comprehensive Cancer Center Hamburg, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. c.bokemeyer@uke.de.
25
Lung Clinic Grosshansdorf, Airway Research Center North, German Center of Lung Research, 22927 Grosshansdorf, Germany. M.Reck@lungenclinic.de.
26
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. s.riethdorf@uke.de.
27
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. pantel@uke.de.
28
Department of Oncology, Hematology and Bone Marrow Transplantation with section Pneumology, Hubertus Wald University Comprehensive Cancer Center Hamburg, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. s.loges@uke.de.
29
Department of Tumor Biology, Center of Experimental Medicine, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany. s.loges@uke.de.

Abstract

Circulating tumor cells (CTCs) hold great potential to answer key questions of how non-small cell lung cancer (NSCLC) evolves and develops resistance upon anti-PD-1/PD-L1 treatment. Currently, their clinical utility in NSCLC is compromised by a low detection rate with the established, Food and Drug Administration (FDA)-approved, EpCAM-based CellSearch® System. We tested an epitope-independent method (ParsortixTM system) and utilized it to assess PD-L1 expression of CTCs from NSCLC patients. We prospectively collected 127 samples, 97 of which were analyzed with the epitope-independent system in comparison to the CellSearch system. CTCs were determined by immunocytochemistry as intact, nucleated, CD45-, pankeratins (K)+ cells. PD-L1 status of CTCs was evaluated from 89 samples. With the epitope-independent system, ≥1 CTC per blood sample was detected in 59 samples (61%) compared to 31 samples (32%) with the EpCAM-based system. Upon PD-L1 staining, 47% of patients harbored only PD-L1+CTCs, 47% had PD-L1+ and PD-L1-CTCs, and only 7% displayed exclusively PD-L1-CTCs. The percentage of PD-L1+CTCs did not correlate with the percentage of PD-L1+ in biopsies determined by immunohistochemistry (p = 0.179). Upon disease progression, all patients showed an increase in PD-L1+CTCs, while no change or a decrease in PD-L1+CTCs was observed in responding patients (n = 11; p = 0.001). Our data show a considerable heterogeneity in the PD-L1 status of CTCs from NSCLC patients. An increase of PD-L1+CTCs holds potential to predict resistance to PD-1/PD-L1 inhibitors.

KEYWORDS:

NSCLC; PD-1/PD-L1 inhibition; circulating tumor cells; resistance

PMID:
31212989
DOI:
10.3390/cancers11060835
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17.
Molecules. 2019 Jun 12;24(12). pii: E2201. doi: 10.3390/molecules24122201.

Introduction of Reversible Urethane Bonds Based on Vanillyl Alcohol for Efficient Self-Healing of Polyurethane Elastomers.

Author information

1
Division of Semiconductor and Chemical Engineering, Chonbuk National University, Baekjedaero 567, Jeonju 54896, Korea. dwlee2310@hanmail.net.
2
Division of Semiconductor and Chemical Engineering, Chonbuk National University, Baekjedaero 567, Jeonju 54896, Korea. hnk07@hanmail.net.
3
Division of Semiconductor and Chemical Engineering, Chonbuk National University, Baekjedaero 567, Jeonju 54896, Korea. daisoolee@jbnu.ac.kr.

Abstract

Urethane groups formed by reacting phenolic hydroxyl groups with isocyanates are known to be reversible at high temperatures. To investigate the intrinsic self-healing of polyurethane via a reversible urethane group, we synthesized vanillyl alcohol (VA)-based polyurethanes. The phenolic hydroxyl group of vanillyl alcohol allows the introduction of a reversible urethane group into the polyurethane backbone. Particularly, we investigated the effects of varying the concentration of reversible urethane groups on the self-healing of the polyurethane, and we proposed a method that improved the mobility of the molecules contributing to the self-healing process. The concentration of reversible urethane groups in the polyurethanes was controlled by varying the vanillyl alcohol content. Increasing the concentration of the reversible urethane group worsened the self-healing property by increasing hydrogen bonding and microphase separation, which consequently decreased the molecular mobility. On the other hand, after formulating a modified chain extender (m-CE), hydrogen bonding and microphase separation decreased, and the mobility (and hence the self-healing efficiency) of the molecules improved. In VA40-10 (40% VA; 10% m-CE) heated to 140 °C, the self-healing efficiency reached 96.5% after 30 min, a 139% improvement over the control polyurethane elastomer (PU). We conclude that the self-healing and mechanical properties of polyurethanes might be tailored for applications by adjusting the vanillyl alcohol content and modifying the chain extender.

KEYWORDS:

mechanical property; reversible urethane bond; self-healing efficiency; vanillyl alcohol

PMID:
31212813
DOI:
10.3390/molecules24122201
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18.
Nutrients. 2019 Jun 12;11(6). pii: E1316. doi: 10.3390/nu11061316.

Aronia Berry Supplementation Mitigates Inflammation in T Cell Transfer-Induced Colitis by Decreasing Oxidative Stress.

Author information

1
Department of Food Science, University of Wisconsin-Madison, 1605 Linden Dr., Madison, WI 53706, USA. ruisong.pei@wisc.edu.
2
Department of Food Science, University of Wisconsin-Madison, 1605 Linden Dr., Madison, WI 53706, USA. jliu678@wisc.edu.
3
China Agricultural University, College of Food Science and Nutritional Engineering, No.17 Qinghua Dong Lu, Beijing 100083, China. jliu678@wisc.edu.
4
Department of Food Science, University of Wisconsin-Madison, 1605 Linden Dr., Madison, WI 53706, USA. mrtn.drk@gmail.com.
5
Department of Food Science, University of Wisconsin-Madison, 1605 Linden Dr., Madison, WI 53706, USA. jcvaldez@wisc.edu.
6
Wisconsin Institutes for Medical Research, University of Wisconsin-Madison, 1111 Highland Ave., Madison, WI 53706, USA. jjjeffery@wisc.edu.
7
Mass Spectrometry Facility, Biotechnology Center, University of Wisconsin-Madison, 425 Henry Mall, Madison, WI 53706, USA. barrettwilt@wisc.edu.
8
University of Massachusetts, Amherst, School of Public Health and Health Sciences, 100 Holdsworth Way, Amherst, MA 01003, USA. zliu@nutrition.umass.edu.
9
Department of Food Science, University of Wisconsin-Madison, 1605 Linden Dr., Madison, WI 53706, USA. bwbolling@wisc.edu.

Abstract

Oxidative stress is involved in the pathogenesis and progression of inflammatory bowel disease. Consumption of aronia berry inhibits T cell transfer colitis, but the antioxidant mechanisms pertinent to immune function are unclear. We hypothesized that aronia berry consumption could inhibit inflammation by modulating the antioxidant function of immunocytes and gastrointestinal tissues. Colitis was induced in recombinase activating gene-1 deficient (Rag1-/-) mice injected with syngeneic CD4+CD62L+ naïve T cells. Concurrent with transfer, mice consumed either 4.5% w/w aronia berry-supplemented or a control diet for five weeks. Aronia berry inhibited intestinal inflammation evidenced by lower colon weight/length ratios, 2-deoxy-2-[18F]fluoro-d-glucose (FDG) uptake, mRNA expressions of tumor necrosis factor alpha (TNF-α), and interferon gamma (IFN-γ) in the colon. Aronia berry also suppressed systemic inflammation evidenced by lower FDG uptake in the spleen, liver, and lung. Colitis induced increased colon malondialdehyde (MDA), decreased colon glutathione peroxidase (GPx) activity, reduced glutathione (rGSH) level, and suppressed expression of antioxidant enzymes in the colon and mesenteric lymph node (MLN). Aronia berry upregulated expression of antioxidant enzymes, prevented colitis-associated depletion of rGSH, and maintained GPx activity. Moreover, aronia berry modulated mitochondria-specific antioxidant activity and decreased splenic mitochondrial H2O2 production in colitic mice. Thus, aronia berry consumption inhibits oxidative stress in the colon during T cell transfer colitis because of its multifaceted antioxidant function in both the cytosol and mitochondria of immunocytes.

KEYWORDS:

adoptive transfer colitis; aronia berry; inflammatory bowel disease; oxidative stress

PMID:
31212794
DOI:
10.3390/nu11061316
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19.
Int J Mol Sci. 2019 Jun 12;20(12). pii: E2859. doi: 10.3390/ijms20122859.

Single Crystal FLIM Characterization of Clofazimine Loaded in Silica-Based Mesoporous Materials and Zeolites.

Author information

1
Departamento de Química Física, Facultad de Ciencias Ambientales y Bioquímica, and INAMOL, Universidad de Castilla-La Mancha, Avenida Carlos III, S/N, 45071 Toledo, Spain. Lorenzo.Angiolini@uclm.es.
2
Departamento de Química Física, Facultad de Ciencias Ambientales y Bioquímica, and INAMOL, Universidad de Castilla-La Mancha, Avenida Carlos III, S/N, 45071 Toledo, Spain. Boyko.Koen@uclm.es.
3
Departamento de Química Física, Facultad de Ciencias Ambientales y Bioquímica, and INAMOL, Universidad de Castilla-La Mancha, Avenida Carlos III, S/N, 45071 Toledo, Spain. abderrazzak.douhal@uclm.es.

Abstract

Clofazimine (CLZ) is an effective antibiotic used against a wide spectrum of Gram-positive bacteria and leprosy. One of its main drawbacks is its poor solubility in water. Silica based materials are used as drug delivery carriers that can increase the solubility of different hydrophobic drugs. Here, we studied how the properties of the silica framework of the mesoporous materials SBA-15, MCM-41, Al-MCM-41, and zeolites NaX, NaY, and HY affect the loading, stability, and distribution of encapsulated CLZ. Time-correlated single-photon counting (TCSPC) and fluorescence lifetime imaging microscopy (FLIM) experiments show the presence of neutral and protonated CLZ (1.3-3.8 ns) and weakly interacting aggregates (0.4-0.9 ns), along with H- and J-type aggregates (<0.1 ns). For the mesoporous and HY zeolite composites, the relative contribution to the overall emission spectra from H-type aggregates is low (<10%), while for the J-type aggregates it becomes higher (~30%). For NaX and NaY the former increased whereas the latter decreased. Although the CLZ@mesoporous composites show higher loading compared to the CLZ@zeolites ones, the behavior of CLZ is not uniform and its dynamics are more heterogeneous across different single mesoporous particles. These results may have implication in the design of silica-based drug carriers for better loading and release mechanisms of hydrophobic drugs.

KEYWORDS:

FLIM; H- and J-aggregates; MCM-41; SBA-15; drug delivery; mesoporous materials; microscopy; silica-based materials; zeolites

PMID:
31212750
DOI:
10.3390/ijms20122859
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20.
Mar Drugs. 2019 Jun 11;17(6). pii: E349. doi: 10.3390/md17060349.

Sulfur-Containing Carotenoids from A Marine Coral Symbiont Erythrobacter flavus Strain KJ5.

Author information

1
Ma Chung Research Center for Photosynthetic Pigments (MRCPP) and Department of Chemistry, Universitas Ma Chung, Villa Puncak Tidar N01, Malang 465151, Indonesia. edi.setiyono@machung.ac.id.
2
Ma Chung Research Center for Photosynthetic Pigments (MRCPP) and Department of Chemistry, Universitas Ma Chung, Villa Puncak Tidar N01, Malang 465151, Indonesia. heri.yanto@machung.ac.id.
3
Department of Coastal Resource Management, Universitas Diponegoro, Jl. Prof. Soedarto Tembalang, Semarang 50275, Indonesia. pringgenies@yahoo.com.
4
Ma Chung Research Center for Photosynthetic Pigments (MRCPP) and Department of Chemistry, Universitas Ma Chung, Villa Puncak Tidar N01, Malang 465151, Indonesia. yshioi08@gmail.com.
5
Research Institute of Green Science and Technology, Shizuoka University, 836 Ohya, Suruga-ku, Shizuoka 422-8529, Japan. kanesaki.yuh@shizuoka.ac.jp.
6
Department of Biological Science, Shizuoka University, 836 Ohya, Suruga-ku, Shizuoka 422-8529, Japan. awai.koichiro@shizuoka.ac.jp.
7
Ma Chung Research Center for Photosynthetic Pigments (MRCPP) and Department of Chemistry, Universitas Ma Chung, Villa Puncak Tidar N01, Malang 465151, Indonesia. tatas.brotosudarmo@machung.ac.id.

Abstract

Erythrobacter flavus strain KJ5 (formerly called Erythrobacter sp. strain KJ5) is a yellowish marine bacterium that was isolated from a hard coral Acropora nasuta in the Karimunjawa Islands, Indonesia. The complete genome sequence of the bacterium has been reported recently. In this study, we examined the carotenoid composition of this bacterium using high-performance liquid chromatography coupled with ESI-MS/MS. We found that the bacterium produced sulfur-containing carotenoids, i.e., caloxanthin sulfate and nostoxanthin sulfate, as the most abundant carotenoids. A new carotenoid zeaxanthin sulfate was detected based on its ESI-MS/MS spectrum. The unique presence of sulfated carotenoids found among the currently known species of the Erythrobacter genus were discussed.

KEYWORDS:

Erythrobacter flavus strain KJ5; caloxanthin sulfate; carotenoids; nostoxanthin sulfate; zeaxanthin sulfate

PMID:
31212714
DOI:
10.3390/md17060349
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