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Journal of Biological Inorganic Chemistry: JBIC

William Keown, J Brannon Gary, T Daniel P Stack
A long-standing debate in the Cu-O2 field has revolved around the relevance of the Cu(III) oxidation state in biological redox processes. The proposal of Cu(III) in biology is generally challenged as no spectroscopic or structural evidence exists currently for its presence. The reaction of synthetic Cu(I) complexes with O2 at low temperature in aprotic solvents provides the opportunity to investigate and define the chemical landscape of Cu-O2 species at a small-molecule level of detail; eight different types are characterized structurally, three of which contain at least one Cu(III) center...
December 1, 2016: Journal of Biological Inorganic Chemistry: JBIC
Xiongyi Huang, John T Groves
Since our initial report in 1976, the oxygen rebound mechanism has become the consensus mechanistic feature for an expanding variety of enzymatic C-H functionalization reactions and small molecule biomimetic catalysts. For both the biotransformations and models, an initial hydrogen atom abstraction from the substrate (R-H) by high-valent iron-oxo species (Fe(n)=O) generates a substrate radical and a reduced iron hydroxide, [Fe(n-1)-OH ·R]. This caged radical pair then evolves on a complicated energy landscape through a number of reaction pathways, such as oxygen rebound to form R-OH, rebound to a non-oxygen atom affording R-X, electron transfer of the incipient radical to yield a carbocation, R(+), desaturation to form olefins, and radical cage escape...
December 1, 2016: Journal of Biological Inorganic Chemistry: JBIC
Emma L Raven
It is well established that there are two different classes of enzymes-tryptophan 2,3-dioxygenase (TDO) and indoleamine 2,3-dioxygenase (IDO)-that catalyse the O2-dependent oxidation of L-tryptophan to N-formylkynurenine. But it was not always so. This perspective presents a short history of the early TDO and IDO literature, the people that were involved in creating it, and the legacy that this left for the future.
December 1, 2016: Journal of Biological Inorganic Chemistry: JBIC
Saliu A Amolegbe, Caroline A Akinremi, Sheriff Adewuyi, Amudat Lawal, Mercy O Bamigboye, Joshua A Obaleye
Metal coordination of bioorganic compounds from both natural and synthetic products is not only gaining recognition in drug design and medicinal inorganic chemistry research, also they are being considered in the improvement of the bioactivity of drugs. What is done in this paper is a review of recent advances in the study of coordination-driven drug delivery, i.e., metal-based drugs (MBDs). The role of some late first row transition metal ions namely Fe, Cu and Zn in the biological activities of metallodrugs such as antimalarials and antimicrobials are highlighted...
November 30, 2016: Journal of Biological Inorganic Chemistry: JBIC
Konstantin B Shumaev, Olga V Kosmachevskaya, Elvira I Nasybullina, Sergey V Gromov, Alexander A Novikov, Alexey F Topunov
Dinitrosyl iron complexes (DNICs) are physiological NO derivatives and account for many NO functions in biology. Polyfunctional dipeptide carnosine (beta-alanyl-L-histidine) is considered to be a very promising pharmacological agent. It was shown that in the system containing carnosine, iron ions and Angeli's salt, a new type of DNICs bound with carnosine as ligand {(carnosine)2-Fe-(NO)2}, was formed. We studied how the carbonyl compound methylglyoxal influenced this process. Carnosine-bound DNICs appear to be one of the cell's adaptation mechanisms when the amount of reactive carbonyl compounds increases at hyperglycemia...
November 22, 2016: Journal of Biological Inorganic Chemistry: JBIC
Matthew O Ross, Amy C Rosenzweig
Methane monooxygenase (MMO) enzymes activate O2 for oxidation of methane. Two distinct MMOs exist in nature, a soluble form that uses a diiron active site (sMMO) and a membrane-bound form with a catalytic copper center (pMMO). Understanding the reaction mechanisms of these enzymes is of fundamental importance to biologists and chemists, and is also relevant to the development of new biocatalysts. The sMMO catalytic cycle has been elucidated in detail, including O2 activation intermediates and the nature of the methane-oxidizing species...
November 22, 2016: Journal of Biological Inorganic Chemistry: JBIC
Raffaella Breglia, Manuel Antonio Ruiz-Rodriguez, Alessandro Vitriolo, Rubén Francisco Gonzàlez-Laredo, Luca De Gioia, Claudio Greco, Maurizio Bruschi
[NiFe]-hydrogenases catalyse the relevant H2 → 2H(+) + 2e(-) reaction. Aerobic oxidation or anaerobic oxidation of this enzyme yields two inactive states called Ni-A and Ni-B. These states differ for the reactivation kinetics which are slower for Ni-A than Ni-B. While there is a general consensus on the structure of Ni-B, the nature of Ni-A is still controversial. Indeed, several crystallographic structures assigned to the Ni-A state have been proposed, which, however, differ for the nature of the bridging ligand and for the presence of modified cysteine residues...
November 21, 2016: Journal of Biological Inorganic Chemistry: JBIC
Ilia A Dereven'kov, Nikita I Shpagilev, László Valkai, Denis S Salnikov, Attila K Horváth, Sergei V Makarov
Reactions of aquacobalamin (H2O-Cbl(III)) and its one-electron reduced form (cob(II)alamin, Cbl(II)) with chlorite (ClO2(-)) and chlorine dioxide (ClO 2(•) ) were studied by conventional and stopped-flow UV-Vis spectroscopies and matrix-assisted laser desorption/ionization-mass spectrometry (MALDI-MS). ClO2(-) does not react with H2O-Cbl(III), but oxidizes Cbl(II) to H2O-Cbl(III) as a major product and corrin-modified species as minor products. The proposed mechanism of chlorite reduction involves formation of OCl(-) that modifies the corrin ring during the course of reaction with Cbl(II)...
November 19, 2016: Journal of Biological Inorganic Chemistry: JBIC
Teresa E Lehmann, Sally A Murray, Azure D Ingersoll, Teresa M Reilly, Shelby E Follett, Kevin E Macartney, Mark H Harpster
The antibiotics known as bleomycins constitute a family of natural products clinically employed for the treatment of a wide spectrum of cancers. The drug acts as an antitumor agent by virtue of the ability of a metal complex of the antibiotic to cleave DNA. Bleomycins are differentiated by their C-terminal regions. Previous structural studies involving metal-bleomycin-DNA triads have allowed the identification of the bithiazole-(C-terminus substituent) segment in this molecule as the one that most closely interacts with DNA...
November 17, 2016: Journal of Biological Inorganic Chemistry: JBIC
Adam T Fiedler, Anne A Fischer
The active sites of metalloenzymes that catalyze O2-dependent reactions generally contain iron or copper ions. However, several enzymes are capable of activating O2 at manganese or nickel centers instead, and a handful of dioxygenases exhibit activity when substituted with cobalt. This minireview summarizes the catalytic properties of oxygenases and oxidases with mononuclear Mn, Co, or Ni active sites, including oxalate-degrading oxidases, catechol dioxygenases, and quercetin dioxygenase. In addition, recent developments in the O2 reactivity of synthetic Mn, Co, or Ni complexes are described, with an emphasis on the nature of reactive intermediates featuring superoxo-, peroxo-, or oxo-ligands...
November 16, 2016: Journal of Biological Inorganic Chemistry: JBIC
Nedjoua Drici, Mohamed Abdelghani Krallafa
Metal-ligand interactions give rise to a wide variety of metal complexes with various physical properties and chemical behaviours and numerous practical applications. The ability of the zinc ion to enhance the structural stability of many proteins by electrostatic interactions or by co-ordination with surrounding amino acids makes it the most important metal ion found in biological systems. In this paper, we highlight the importance of non-covalent interaction established between a metal ion and its environment in stabilizing biomolecules...
November 15, 2016: Journal of Biological Inorganic Chemistry: JBIC
Duygu İnci, Rahmiye Aydın, Özgür Vatan, Tuba Sevgi, Dilek Yılmaz, Yunus Zorlu, Yusuf Yerli, Bünyemin Çoşut, Elif Demirkan, Nilüfer Çinkılıç
New copper(II) complexes-dimeric-[Cu(nphen)(gly)(H2O)](+) (1) and [Cu(dmphen)(gly)(NO3)(H2O)] (2) (nphen = 5-nitro-1,10-phenanthroline, dmphen = 4,7-dimethyl-1,10-phenanthroline, and gly = glycine)-have been synthesized and characterized by CHN analysis, single-crystal X-ray diffraction techniques, FTIR, EPR spectroscopy, and cyclic voltammetry. The CT-DNA-binding properties of these complexes have been investigated by thermal denaturation measurements and both absorption and emission spectroscopy. The DNA cleavage activity of these complexes has been studied on supercoiled pUC19 plasmid DNA by gel electrophoresis experiments in the absence and presence of H2O2...
November 10, 2016: Journal of Biological Inorganic Chemistry: JBIC
Federica Sinibaldi, Lisa Milazzo, Barry D Howes, Maria Cristina Piro, Laura Fiorucci, Fabio Polticelli, Paolo Ascenzi, Massimo Coletta, Giulietta Smulevich, Roberto Santucci
Cytochrome c undergoes structural variations upon binding of cardiolipin, one of the phospholipids constituting the mitochondrial membrane. Although several mechanisms governing cytochrome c/cardiolipin (cyt c/CL) recognition have been proposed, the interpretation of the process remains, at least in part, unknown. To better define the steps characterizing the cyt c-CL interaction, the role of Lys72 and Lys73, two residues thought to be important in the protein/lipid binding interaction, were recently investigated by mutagenesis...
November 9, 2016: Journal of Biological Inorganic Chemistry: JBIC
Manojkumar Jadhao, Chayan Das, Anoop Rawat, Himank Kumar, Ritika Joshi, Sudipta Maiti, Sujit Kumar Ghosh
Amyloid-β peptides and their metal-associated aggregated states have been implicated in the pathogenesis of Alzheimer's disease. The present paper epitomises the design and synthesis of a small, neutral, lipophilic benzothiazole Schiff base (E)-2-((6-chlorobenzo[d]thiazol-2-ylimino)methyl)-5-diethylamino)phenol (CBMDP), and explores its multifunctionalty as a potential metal chelator/fluorophore using UV-visible absorption, steady-state fluorescence, single molecule fluorescence correlation spectroscopic (FCS) techniques which is further corroborated by in silico studies...
November 7, 2016: Journal of Biological Inorganic Chemistry: JBIC
Alexandra S Alves, Nazua L Costa, Ming Tien, Ricardo O Louro, Catarina M Paquete
Dissimilatory metal-reducing bacteria perform extracellular electron transfer, a metabolic trait that is at the core of a wide range of biotechnological applications. To better understand how these microorganisms transfer electrons from their metabolism to an extracellular electron acceptor, it is necessary to characterize in detail the key players in this process, the multiheme c-type cytochromes. Shewanella oneidensis MR-1 is a model organism for studying extracellular electron transfer, where the heme protein referred to as small tetraheme cytochrome is one of the most abundant multiheme cytochromes found in the periplasmic space of this bacterium...
November 5, 2016: Journal of Biological Inorganic Chemistry: JBIC
Fabricio Ragone, Héctor H Martínez Saavedra, Pablo F García, Ezequiel Wolcan, Gerardo A Argüello, Gustavo T Ruiz
A new synthetic route to acquire the water soluble complex fac-Re(I)(CO)3(pterin)(H2O) was carried out in aqueous solution. The complex has been obtained with success via the fac-[Re(I)(CO)3(H2O)3]Cl precursor complex. Re(I)(CO)3(pterin)(H2O) has been found to bind strongly with bovine and human serum albumins (BSA and HSA) with intrinsic-binding constants, Kb, of 6.5 × 10(5) M(-1) and 5.6 × 10(5) M(-1) at 310 K, respectively. The interactions of serum albumins with Re(I)(CO)3(pterin)(H2O) were evaluated employing UV-vis fluorescence and absorption spectroscopy and circular dichroism...
November 4, 2016: Journal of Biological Inorganic Chemistry: JBIC
Denis A Proshlyakov, John McCracken, Robert P Hausinger
A wide range of spectroscopic approaches have been used to interrogate the mononuclear iron metallocenter in 2-oxoglutarate (2OG)-dependent oxygenases. The results from these spectroscopic studies have provided valuable insights into the structural changes at the active site during substrate binding and catalysis, thus providing critical information that complements investigations of these enzymes by X-ray crystallography, biochemical, and computational approaches. This mini-review highlights taurine hydroxylase (taurine:2OG dioxygenase, TauD) as a case study to illustrate the wealth of knowledge that can be generated by applying a diverse array of spectroscopic investigations to a single enzyme...
November 3, 2016: Journal of Biological Inorganic Chemistry: JBIC
Elizabeth M Thomas, Stephen M Testa
Colorimetric methods combined with color-changing chemical probes are widely used as simple yet effective tools for identifying and quantifying a wide variety of molecules in solution. For nucleic acids (DNA and RNA), perhaps the most commonly used colorimetric probe is potassium permanganate, which can be used to identify single-stranded pyrimidines (thymine and cytosine) in polymers. Unfortunately, permanganate is not an effective probe for identifying purines (adenine and guanine), especially in the presence of the more reactive pyrimidines...
November 2, 2016: Journal of Biological Inorganic Chemistry: JBIC
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November 1, 2016: Journal of Biological Inorganic Chemistry: JBIC
Cheng Zhang, Shang-Hai Lai, Chuan-Chuan Zeng, Bing Tang, Dan Wan, De-Gang Xing, Yun-Jun Liu
A new ligand BTCP and its iridium(III) complex [Ir(ppy)2(BTCP)]PF6 (Ir-1) were synthesized and characterized by elemental analysis, ESI-MS, IR, (1)H NMR and (13)C NMR. The cytotoxic activity in vitro of the ligand and its complex against SGC-7901, HeLa, HOS, PC-12, BEL-7402, MG-63, SiHa, A549, HepG2 and normal cell LO2 were evaluated by MTT method [MTT = (3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide)]. The apoptosis was assayed with AO/EB and Hoechst 33258 staining methods. The reactive oxygen species (ROS), mitochondrial membrane potential, autophagy and cell invasion were studied under fluorescent microscope...
October 28, 2016: Journal of Biological Inorganic Chemistry: JBIC
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