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Journal of Biological Inorganic Chemistry: JBIC

Joana Efua Aggrey-Fynn, Nur Basak Surmeli
Hemoproteins are commonly found in nature, and involved in many important cellular processes such as oxygen transport, electron transfer, and catalysis. Rational design of hemoproteins can not only inspire novel biocatalysts but will also lead to a better understanding of structure-function relationships in native hemoproteins. Here, the heme nitric oxide/oxygen-binding protein from Caldanaerobacter subterraneus subsp. tengcongensis (TtH-NOX) is used as a novel scaffold for oxidation biocatalyst design. We show that signaling protein TtH-NOX can be reengineered to catalyze H2 O2 decomposition and oxidation of 2,2'-azino-bis(3-ethylbenzothiazoline-6-sulphonic acid) by H2 O2 ...
September 12, 2018: Journal of Biological Inorganic Chemistry: JBIC
G Y Sánchez Delgado, D Paschoal, H F Dos Santos
Gold complexes are promising compounds used in cancer chemotherapy. Besides their steric features, which enable biomolecule interactions, the redox instability and the high affinity of gold with cellular nucleophiles influence the biological action in these complexes. Both features were herein theoretically investigated for the [Au(C^N^C)Cl] probe complex (C^N^C = 2,6-diphenylpyridine) using H2 O, CH3 SH/CH3 S- , CH3 Se- and meim-4-H (4-methylimidazole) as biomimetic nucleophiles. Based on the results, the lowest energy reaction path followed two consecutive steps: (1) chloride-exchange ([Formula: see text] = 4...
September 12, 2018: Journal of Biological Inorganic Chemistry: JBIC
Geoffrey A Heinzl, Weiliang Huang, Elizabeth Robinson, Fengtian Xue, Pierre Möenne-Loccoz, Angela Wilks
The P. aeruginosa iron-regulated heme oxygenase (HemO) is required within the host for the utilization of heme as an iron source. As iron is essential for survival and virulence, HemO represents a novel antimicrobial target. We recently characterized small molecule inhibitors that bind to an allosteric site distant from the heme pocket, and further proposed binding at this site disrupts a nearby salt bridge between D99 and R188. Herein, through a combination of site-directed mutagenesis and hydrogen-deuterium exchange mass spectrometry (HDX-MS), we determined that the disruption of the D99-R188 salt bridge leads to significant decrease in conformational flexibility within the distal and proximal helices that form the heme-binding site...
September 8, 2018: Journal of Biological Inorganic Chemistry: JBIC
Gonzalo Scalese, Ignacio Machado, Carolina Fontana, Gastón Risi, Gustavo Salinas, Leticia Pérez-Díaz, Dinorah Gambino
Searching for prospective vanadium-based agents against Trypanosoma cruzi, the parasite causing Chagas disease, four new [VV O(8HQ-H)(L-2H)] compounds, where 8HQ is 8-hydroxyquinoline and L are tridentate salicylaldehyde semicarbazone derivatives L1-L4, were synthesized and characterized in the solid state and in solution. The compounds were evaluated on T. cruzi epimastigotes (CL Brener) as well as on VERO cells, as mammalian cell model. Compounds showed activity against T. cruzi (IC50 6.2-10.5 μM) of the same order than Nifurtimox and 8HQ, and a four- to sevenfold activity increase with respect to the free semicarbazones...
September 8, 2018: Journal of Biological Inorganic Chemistry: JBIC
Sriramya Garapati, William Monteith, Chris Wilson, Anastasiia Kostenko, John M Kenney, Allison S Danell, Colin S Burns
Prothymosin-α is a small, multifunctional intrinsically disordered protein associated with cell survival and proliferation which binds multiple Zn2+ ions and undergoes partial folding. The interaction between prothymosin-α and at least two of its protein targets is significantly enhanced in the presence of Zn2+ ions, suggesting that Zn2+ binding plays a role in the protein's function. The primary sequence of prothymosin-α is highly acidic, with almost 50% comprised of Asp and Glu, and is unusual for a Zn2+ -binding protein as it lacks Cys and His residues...
September 5, 2018: Journal of Biological Inorganic Chemistry: JBIC
Geng Dong, Ulf Ryde
Formate dehydrogenases (FDHs) are metalloenzymes that catalyse the reversible conversion of formate to carbon dioxide. Since such a process may be used to combat the greenhouse effect, FDHs have been extensively studied by experimental and theoretical methods. However, the reaction mechanism is still not clear; instead five putative mechanisms have been suggested. In this work, the reaction mechanism of FDH was studied by computational methods. Combined quantum mechanical and molecular mechanic (QM/MM) optimisations were performed to obtain the geometries...
September 1, 2018: Journal of Biological Inorganic Chemistry: JBIC
J A Domínguez-Calva, M L Pérez-Vázquez, E Serebryany, J A King, L Quintanar
Cataract disease results from non-amyloid aggregation of eye lens proteins and is the leading cause of blindness in the world. A variety of studies have implicated both essential and xenobiotic metals as potential etiological agents in cataract disease. Essential metal ions, such as copper and zinc, are known to induce the aggregation in vitro of human γD crystallin, one of the more abundant γ-crystallins in the core of the lens. In this study, we expand the investigation of metal-crystallin interactions to heavy metal ions, such as divalent lead, cadmium and mercury...
August 30, 2018: Journal of Biological Inorganic Chemistry: JBIC
Daphne S Cukierman, Elio Accardo, Rosana Garrido Gomes, Anna De Falco, Marco C Miotto, Maria Clara Ramalho Freitas, Mauricio Lanznaster, Claudio O Fernández, Nicolás A Rey
With the increasing life expectancy of the world's population, neurodegenerative diseases, such as Alzheimer's disease (AD), will become a much more relevant public health issue. This fact, coupled with the lack of efficacy of the available treatments, has been driving research directed to the development of new drugs for this pathology. Metal-protein attenuating compounds (MPACs) constitute a promising class of agents with potential application on the treatment of neurodegenerative diseases, such as AD. Currently, most MPACs are based on 8-hydroxyquinoline...
August 25, 2018: Journal of Biological Inorganic Chemistry: JBIC
Jesse G Kleingardner, Benjamin D Levin, Giorgio Zoppellaro, K Kristoffer Andersson, Sean J Elliott, Kara L Bren
Heme c is characterized by its covalent attachment to a polypeptide. The attachment is typically to a CXXCH motif in which the two Cys form thioether bonds with the heme, "X" can be any amino acid other than Cys, and the His serves as a heme axial ligand. Some cytochromes c, however, contain heme attachment motifs with three or four intervening residues in a CX3 CH or CX4 CH motif. Here, the impacts of these variations in the heme attachment motif on heme ruffling and electronic structure are investigated by spectroscopically characterizing CX3 CH and CX4 CH variants of Hydrogenobacter thermophilus cytochrome c552 ...
August 24, 2018: Journal of Biological Inorganic Chemistry: JBIC
Michael Rohde, Christian Trncik, Daniel Sippel, Stefan Gerhardt, Oliver Einsle
Nitrogenases catalyze the biological fixation of inert N2 into bioavailable ammonium. They are bipartite systems consisting of the catalytic dinitrogenase and a complementary reductase, the Fe protein that is also the site where ATP is hydrolyzed to drive the reaction forward. Three different subclasses of dinitrogenases are known, employing either molybdenum, vanadium or only iron at their active site cofactor. Although in all these classes the mode and mechanism of interaction with Fe protein is conserved, each one encodes its own orthologue of the reductase in the corresponding gene cluster...
August 23, 2018: Journal of Biological Inorganic Chemistry: JBIC
Hiroaki Naka, Zachary L Reitz, Aneta L Jelowicki, Alison Butler, Margo G Haygood
Vibrio campbellii BAA-1116 (formerly Vibrio harveyi) is a model organism for quorum sensing study and produces the siderophores anguibactin and amphi-enterobactin. This study examined the mechanisms and specificity of siderophore uptake in V. campbellii and V. harveyi, and surveyed the diversity of siderophore production in V. campbellii and V. harveyi strains. The amphi-enterobactin gene cluster of BAA-1116 harbors a gene, named fapA, that is a homologue of genes encoding Fe(III)-siderophore-specific outer membrane receptors...
August 22, 2018: Journal of Biological Inorganic Chemistry: JBIC
Yue Wen Deng, Soo Y Ro, Amy C Rosenzweig
In methylotrophic bacteria, which use one-carbon (C1) compounds as a carbon source, methanol is oxidized by pyrroloquinoline quinone (PQQ)-dependent methanol dehydrogenase (MDH) enzymes. Methylotrophic genomes generally encode two distinct MDHs, MxaF and XoxF. MxaF is a well-studied, calcium-dependent heterotetrameric enzyme whereas XoxF is a lanthanide-dependent homodimer. Recent studies suggest that XoxFs are likely the functional MDHs in many environments. In methanotrophs, methylotrophs that utilize methane, interactions between particulate methane monooxygenase (pMMO) and MxaF have been detected...
August 21, 2018: Journal of Biological Inorganic Chemistry: JBIC
Cecilia Pozzi, Flavio Di Pisa, Manuela Benvenuti, Stefano Mangani
Recent evidence links the role of human glutaminyl cyclase (hQC) to the amyloidogenic process involved in Alzheimer's disease (AD). hQC is a zinc enzyme present in neuronal tissue and its activity is responsible for the cyclization of N-terminal Gln or Glu β-amyloid peptides, leading to N-pyroglutamic acid peptides (pE-Aβ) that is probably a crucial event in the initiation and progress of the disease. Indeed, pE-containing peptides exhibit an elevated neurotoxicity and a tendency to aggregate. These observations render hQC inhibition an attractive strategy for developing new molecules active against AD...
August 21, 2018: Journal of Biological Inorganic Chemistry: JBIC
Gudepalya Renukaiah Rudramurthy, Mallappa Kumara Swamy
Nanotechnology advancements have led to the development of its allied fields, such as nanoparticle synthesis and their applications in the field of biomedicine. Nanotechnology driven innovations have given a hope to the patients as well as physicians in solving the complex medical problems. Nanoparticles with a size ranging from 0.2 to 100 nm are associated with an increased surface to volume ratio. Moreover, the physico-chemical and biological properties of nanoparticles can be modified depending on the applications...
August 10, 2018: Journal of Biological Inorganic Chemistry: JBIC
Víctor A Barrera-Guzmán, Edgar O Rodríguez-Hernández, Naytzé Ortíz-Pastrana, Ricardo Domínguez-González, Ana B Caballero, Patrick Gamez, Norah Barba-Behrens
Four copper(II) coordination compounds from 2-benzimidazole propionic acid (Hbzpr) and 4-(benzimidazol-2-yl)-3-thiobutanoic acid (Hbztb) were synthesized and fully characterized by elemental analyses, electronic spectroscopy, FT-IR and mass spectrometry. The molecular structure for the four complexes was confirmed by single-crystal X-ray crystallography. The DNA-interacting properties of the two trinuclear and two mononuclear compounds were investigated using different spectroscopic techniques including absorption titration experiments, fluorescence spectroscopy and circular dichroism spectroscopy...
August 3, 2018: Journal of Biological Inorganic Chemistry: JBIC
Alexey A Nazarov, Maria-Grazia Mendoza-Ferri, Muhammad Hanif, Bernhard K Keppler, Paul J Dyson, Christian G Hartinger
The dinuclear anticancer agents 1,n-bis{chlorido[3-(oxo-κO)-2-methyl-4-(1H)-pyridinonato-κO4](η6 -p-cymene)-ruthenium(II)}alkane (PyRu 2 n ) exhibit high antiproliferative activity in human cancer cell. Reactivity studies with DNA and protein revealed uncommon protein-DNA and DNA-DNA crosslinking ability. We report here studies on the reactions of the diruthenium organometallics PyRu 2 6 and PyRu 2 8 in comparison with a mononuclear analogue PyRu3 with amino acids using mass spectrometry and NMR spectroscopy...
July 25, 2018: Journal of Biological Inorganic Chemistry: JBIC
Floyd A Beckford, Madison B Niece, Brittany P Lassiter, Stephen J Beebe, Alvin A Holder
It is now well established that ruthenium complexes are attractive alternatives to platinum-based anticancer agents. Most of the ruthenium compounds currently under investigation contain a single metal center. The synthesis of multinuclear analogues may provide access to novel complexes with enhanced biological activity. In this work, we have synthesized a set of three trinuclear complexes containing organometallic ruthenium fragments-(arene)RuCl-coordinated to a 2,4,6-tris(di-2-pyridylamino)-1,3,5-triazine core [(Arene = benzene (2), p-cymene (1), or hexamethylbenzene (3)]...
July 23, 2018: Journal of Biological Inorganic Chemistry: JBIC
Courtney F McQueen, John T Groves
The complex stability constant (log β110 ) and the free iron concentration (pM) are used to compare the relative strength of iron binding by siderophores. Direct measurements of these thermodynamic parameters are often not possible for siderophores due to very large log β110 values ranging from 30 to 50. Instead, siderophore iron(III)-binding constants are determined by competitive experiments with other strong chelators with known values, such as EDTA. Iron(III) binding constants of water-insoluble siderophores, such as the mycobactins produced by the mycobacterium family, have never been directly measured...
July 16, 2018: Journal of Biological Inorganic Chemistry: JBIC
Moumita Mukherjee, Pinki Saha Sardar, Pritam Roy, Swagata Dasgupta, Maitrayee Basu Roy, Sanjib Ghosh
A ternary system comprising of a Eu(III) complex of the drug Tetracycline hydrochloride (Eu3 TC) bound to bovine β-lactoglobulin variant A (BLGA) in aqueous buffer at physiological pH (pH = 7.4) has been investigated to exploit the enhanced "antenna effect" to locate the bound drug and find the microenvironment of the binding site. Steady-state and time-resolved emission studies at room temperature as well as at 77 K have been carried out to evaluate the binding parameters in the binary system consisting of BLGA and tetracycline hydrochloride (TC)...
July 13, 2018: Journal of Biological Inorganic Chemistry: JBIC
Fang Xie, Huawei Cai, Fangyu Peng
Copper 8-hydroxyquinoline-2-carboxaldehyde-thiosemicarbazide complex (CuHQTS) is a copper complex with strong anticancer activity against cisplatin-resistant neuroblastoma and prostate cancer cells in vitro by cell proliferation assay or fluorescent microscopic imaging. This study aimed to evaluate anti-prostate cancer activity of CuHQTS in vivo by bioluminescence imaging (BLI) and tumor size measurement, using athymic nu/nu mice implanted with prostate cancer cells carrying luciferase reporter gene (Luc-PC3)...
July 13, 2018: Journal of Biological Inorganic Chemistry: JBIC
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