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91.
Scarpellini M Gätjens J Martin OJ Kampf JW Sherman SE Pecoraro VL 《Inorganic chemistry》2008,47(9):3584-3593
In view of the biological and commercial interest in models for Oxalate Decarboxylases (OxDC) and Oxalate Oxidases (OxOx), we have synthesized and characterized three new Mn (II) complexes ( 1- 3) employing N3O-donor amino-carboxylate ligands (TCMA, 1,4,7-triazacyclononane- N-acetic acid; K (i) Pr 2TCMA, potassium 1,4-diisopropyl-1,4,7-triazacyclononane- N-acetate; and KBPZG, potassium N,N-bis(3,5-dimethylpyrazolyl methyl)glycinate). These complexes were characterized by several techniques including X-ray crystallographic analysis, X-band electron paramagnetic resonance (EPR), electrospray ionization mass spectrometry (ESI-MS), and cyclic voltammetry. The crystal structures of 1 and 3 revealed that both form infinite polymeric chains of Mn (II) complexes linked by the pendant carboxylate arms of the TCMA (-) and the BPZG (-) ligands in a syn-antipattern. Complex 2 crystallizes as a mononuclear Mn (II) cation, six-coordinate in a distorted octahedral geometry. Although complexes 1 and 3 crystallize as polymeric chains, all compounds present the same N3O-donor set atoms around the metal center as observed in the crystallographically characterized OxDC and OxOx. Moreover, complex 2 also contains two water molecules coordinated to the Mn center as observed in the active site of OxDC and OxOx. ESI-MS spectrometry, combined with EPR, were useful techniques to establish that complexes 1- 3 are present as mononuclear Mn (II) species in solution. Finally, complexes 1- 3 are able to model the resting state active sites, with special attention focused on complex 2 which provides the first exact first coordination sphere ligand structural model for the resting states of both OxDC and OxOx. 相似文献
92.
Disinfection and Mechanistic Insights of Escherichia coli in Water by Bismuth Oxyhalide Photocatalysis 下载免费PDF全文
Ilana Sherman Yoram Gerchman Yoel Sasson Hani Gnayem Hadas Mamane 《Photochemistry and photobiology》2016,92(6):826-834
This study demonstrates the potential of a new BiOCl0.875Br0.125 photocatalyst to disinfect Escherichia coli in water under simulated solar irradiation. Photocatalytic efficiency was examined for different photocatalyst loadings, solar wavelengths, exposure times, photocatalyst concentration × contact time (Ct) concept and with the use of scavengers. To elucidate the inactivation mechanism, we examined DNA damage, membrane damage, lipid peroxidation and protein release. Both photolysis and photocatalysis were negligible under visible irradiation, but enhanced photocatalytic activity was observed under solar UVA (λ > 320 nm) and UVB (λ > 280 nm), with 1.5 and 3.6 log inactivation, respectively, after 40 min of irradiation. The log inactivation vs Ct curve for E. coli by UVA/BiOCl0.875Br0.125 was fairly linear, with Ct = 10 g L?1 × min, resulting in 2 log inactivation. Photocatalytic treatment led to membrane damage, but without lipid peroxidation. Accordingly, protein was released from the cells after UVA or UVA/BiOCl0.875Br0.125 treatment. Photocatalysis also increased endonuclease‐sensitive sites vs photolysis alone, by an unknown mechanism. Finally, E. coli inactivation was not influenced by the addition of tert‐butanol or l ‐histidine, implying that neither hydroxyl radicals nor singlet oxygen reactive species are involved in the inactivation process. 相似文献
93.
94.
V. I. Medvedev A. A. Vasiliev K. N. Ermakov V. P. Koptev L. M. Kochenda V. I. Poromov O. V. Rogachevsky V. V. Sarantsev V. A. Trofimov S. G. Sherman 《Physics of Atomic Nuclei》2009,72(9):1475-1478
The energy spectrum of a neutron beam produced in a thin-wall liquid-deuterium target by a proton beam of energy 1 GeV was
measured in a hydrogen bubble chamber by detecting events of the reaction np → ppπ
−. 相似文献
95.
96.
K. N. Ermakov V. I. Medvedev V. A. Nikonov O. V. Rogachevsky A. V. Sarantsev V. V. Sarantsev S. G. Sherman 《The European Physical Journal A - Hadrons and Nuclei》2014,50(6):1-6
The new data on the elastic pp and single-pion production reaction pp → pnπ + taken at the incident proton momentum 1581 MeV/c are presented. To extract contributions of the leading partial waves the single-pion production data are analyzed in the framework of the event-by-event maximum-likelihood method together with pp → ppπ + data measured earlier and the pp → pnπ + data taken at 1628 MeV/c. The analysis shows that at 1581 MeV/c the largest contributions stem from the 3 P 2, 3 P 1, 3 P 0 and 3 F 2 initial partial waves. From these partial waves we also deduce contributions for the production of the Δ(1232) and N(1440) states. 相似文献
97.
JO Freeman ME Murphy JC Sherman 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(36):11409-11416
We have reported a template assembled synthetic protein (cavitein?Q4) as an unexpected dimer in the solid state and as a monomer-dimer equilibrium in solution. We have since reported an ability to bias a cavitein's monomer-dimer equilibrium in solution by sequence design involving histidine metal chelation or disulfide incorporation. However, little remains known about the forces contributing to dimeric cavitein crystal nucleation and lattice stabilization. We, therefore, designed glutamine variants to probe factors involved in dimeric cavitein crystallization. It was found that a key glutamate hydrogen-bonding interaction between dimers is integral to crystal formation and stabilization. Additionally, we obtained a crystal structure of a cavitein (Q4-E3H) designed to bias the dimeric structure via histidine metal coordination. The resolved structure indicates a histidine cluster interaction that likely accounts for the biased dimeric form observed in solution. 相似文献
98.
Finefield JM Sherman DH Kreitman M Williams RM 《Angewandte Chemie (International ed. in English)》2012,51(20):4802-4836
In nature, chiral natural products are usually produced in optically pure form-however, occasionally both enantiomers are formed. These enantiomeric natural products can arise from a single species or from different genera and/or species. Extensive research has been carried out over the years in an attempt to understand the biogenesis of naturally occurring enantiomers; however, many fascinating puzzles and stereochemical anomalies still remain. 相似文献
99.
Chemler JA Buchholz TJ Geders TW Akey DL Rath CM Chlipala GE Smith JL Sherman DH 《Journal of the American Chemical Society》2012,134(17):7359-7366
Germicidin synthase (Gcs) from Streptomyces coelicolor is a type III polyketide synthase (PKS) with broad substrate flexibility for acyl groups linked through a thioester bond to either coenzyme A (CoA) or acyl carrier protein (ACP). Germicidin synthesis was reconstituted in vitro by coupling Gcs with fatty acid biosynthesis. Since Gcs has broad substrate flexibility, we directly compared the kinetic properties of Gcs with both acyl-ACP and acyl-CoA. The catalytic efficiency of Gcs for acyl-ACP was 10-fold higher than for acyl-CoA, suggesting a strong preference toward carrier protein starter unit transfer. The 2.9 ? germicidin synthase crystal structure revealed canonical type III PKS architecture along with an unusual helical bundle of unknown function that appears to extend the dimerization interface. A pair of arginine residues adjacent to the active site affect catalytic activity but not ACP binding. This investigation provides new and surprising information about the interactions between type III PKSs and ACPs that will facilitate the construction of engineered systems for production of novel polyketides. 相似文献
100.
Aqueous room temperature synthesis of cobalt and zinc sodalite zeolitic imidizolate frameworks 总被引:1,自引:0,他引:1
Sodalite zeolitic imidazolate frameworks containing Co (ZIF-67) and Zn (ZIF-8) were synthesized at room temperature under aqueous conditions in 10 min. A trialkylamine deprotonated the 2-methylimidazole ligand and nucleated the frameworks. Furthermore, the ligand acted as a structure directing agent in place of an organic solvent. 相似文献