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Joanna Borowiec, William P Gillin, Maureen A C Willis, Filippo S Boi, Y He, J Q Wen, S L Wang, Leander Schulz
In this study, a direct sulfidation reaction of ammonium perrhenate (NH4ReO4) leading to a synthesis of rhenium disulfide (ReS2) is demonstrated. These findings reveal the first example of a simplistic bottom-up approach to the chemical synthesis of crystalline ReS2. The reaction presented here takes place at room temperature, in an ambient and solvent-free environment and without the necessity of a catalyst. The atomic composition and structure of the as-synthesized product were characterized using several analysis techniques including energy dispersive x-ray spectroscopy, x-ray photoelectron spectroscopy, x-ray diffraction, transmission electron microscopy, Raman spectroscopy, thermogravimetric analysis and differential scanning calorimetry...
January 11, 2018: Journal of Physics. Condensed Matter: An Institute of Physics Journal
Sierra C Marker, Samantha N MacMillan, Warren R Zipfel, Zhi Li, Peter C Ford, Justin J Wilson
Fifteen water-soluble rhenium compounds of the general formula [Re(CO)3(NN)(PR3)]+, where NN is a diimine ligand and PR3 is 1,3,5-triaza-7-phosphaadamantane (PTA), tris(hydroxymethyl)phosphine (THP), or 1,4-diacetyl-1,3,7-triaza-5-phosphabicylco[3.3.1]nonane (DAPTA), were synthesized and characterized by multinuclear NMR spectroscopy, IR spectroscopy, and X-ray crystallography. The complexes bearing the THP and DAPTA ligands exhibit triplet-based luminescence in air-equilibrated aqueous solutions with quantum yields ranging from 3...
January 11, 2018: Inorganic Chemistry
Wenlong Zhang, Guoying Deng, Bo Li, Xinxin Zhao, Tao Ji, Guosheng Song, Zhiyin Xiao, Qing Cao, Jingbo Xiao, Xiaojuan Huang, Guoqiang Guan, Rujia Zou, Xinwu Lu, Junqing Hu
The applications of inorganic theranostic agents in clinical trials are generally limited to their innate non-biodegradability and potential long-term biotoxicity. To address this problem, herein via a straightforward and tailored space-confined on-substrate route, we obtained rhenium trioxide (ReO3) nanocubes (NCs) that display a good biocompatibility and biosafety. Importantly, their aqueous dispersion has high localized surface plasmon resonance (LSPR) absorbance in near-infrared (NIR) region different from previous report, which possibly associates with the charge transfer and structural distortion in hydrogen rhenium bronze (HxReO3), as well as ReO3's cubic shape...
December 27, 2017: Biomaterials
Jani Hämäläinen, Miika Mattinen, Kenichiro Mizohata, Kristoffer Meinander, Marko Vehkamäki, Jyrki Räisänen, Mikko Ritala, Markku Leskelä
2D materials research is advancing rapidly as various new "beyond graphene" materials are fabricated, their properties studied, and materials tested in various applications. Rhenium disulfide is one of the 2D transition metal dichalcogenides that has recently shown to possess extraordinary properties such as that it is not limited by the strict monolayer thickness requirements. The unique inherent decoupling of monolayers in ReS2 combined with a direct bandgap and highly anisotropic properties makes ReS2 one of the most interesting 2D materials for a plethora of applications...
January 5, 2018: Advanced Materials
Xiaoyang Zhang, Yaqin Hou, Cheng Peng, Chu Wang, Xiang Wang, Zhigang Liang, Jing Lu, Baian Chen, Jiapei Dai, Boli Liu, Mengchao Cui
Oligoethyleneoxy linker was introduced for conjugation between 99mTc/Re-bis(aminoethanethiol) (BAT) and β-amyloid (Aβ) binding scaffolds. Rhenium complexes exhibited high to medium binding affinity to Aβ1-42 aggregates and efficient fluorescent staining to Aβ plaques in brain tissue. After radiolabeling, the 99mTc-labeled probes revealed improved brain pharmacokinetics in biodistribution study on normal ICR mice. Probe [99mTc]15 with potent binding affinity (Ki = 13.4 nM) and highest initial brain uptake (2...
January 5, 2018: Journal of Medicinal Chemistry
Michelle Muñoz-Osses, Fernando Godoy, Angélica Fierro, Alejandra Gómez, Nils Metzler-Nolte
Substituted amino-piperazine derivatives were synthesized and used as precursors for the preparation of a series of new organometallic Re(i) imine complexes with the general formula [(η5-C5H4CH[double bond, length as m-dash]N-(CH2)5-Pz-R)Re(CO)3] (Pz-R: -alkyl or aryl piperazine). The piperazine-based ligands were designed to be potential inhibitors of GSK-3β kinase. All the ligands and complexes were fully characterized and evaluated against the HT-29 and PT-45 cancer cell lines, in which GSK-3β plays a crucial role...
January 4, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
Joanna Borowiec, William P Gillin, Maureen Willis, Filippo Boi, Yi He, Jiqiu Wen, Shanling Wang, Leander Schulz
In this study, a direct sulfidation reaction of ammonium perrhenate (NH<sub>4</sub>ReO<sub>4</sub>) leading to a synthesis of rhenium disulfide (ReS<sub>2</sub>) is demonstrated. These finding reveal the first example of a simplistic bottom-up approach to the chemical synthesis of crystalline ReS<sub>2</sub>. The reaction presented here takes place at room temperature, in an ambient and solvent-free environment and without the necessity of a catalyst. The atomic composition and structure of the as-synthesized product were characterized using several analysis techniques including energy dispersive X-ray (EDX) spectroscopy, X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), transmission electron microscopy (TEM), Raman spectroscopy, thermogravimetric analysis (TGA) and differential scannig calorimetry (DSC)...
December 29, 2017: Journal of Physics. Condensed Matter: An Institute of Physics Journal
Saray Argibay-Otero, Rosa Carballo, Ezequiel M Vázquez-López
The asymmetric unit of the title compound, [ReCl(C5H5NO)2(CO)3]·C5H5NO, contains one mol-ecule of the complex fac-[ReCl(4-pyOH)2(CO)3] (where 4-pyOH represents 4-hy-droxy-pyridine) and one mol-ecule of pyridin-4(1H)-one (4-HpyO). In the mol-ecule of the complex, the Re atom is coordinated to two N atoms of the two 4-pyOH ligands, three carbonyl C atoms, in a facial configuration, and the Cl atom. The resulting geometry is slightly distorted octa-hedral. In the crystal structure, both fragments are associated by hydrogen bonds; two 4-HpyO mol-ecules bridge between two mol-ecules of the complex using the O=C group as acceptor for two different HO- groups of coordinated 4-pyOH from two neighbouring metal complexes...
October 1, 2017: Acta Crystallographica. Section E, Crystallographic Communications
Nikola S Lambic, Roger D Sommer, Elon A Ison
The synthesis of (PNP)Re(N)X (PNP = [2-P(CHMe2)2-4-MeC6H3]2N, X = Cl and Me) complexes is described. The methylnitridorhenium complex 3 was found to react differently with CO and isocyanides, leading to the isolation of a Re(v) acyl complex 4 and an isocyanide adduct 6. Two parallel pathways were observed for the reaction of 3 with CO: (1) CO inserts into the Re-Me bond to afford 4, and (2) 3 isomerizes by distortion of the aryl backbone of the PNP ligand to afford the isomer 3'. This is followed by the reaction of 3' with CO to afford the tricarbonyl complex 5, which was fully characterized...
December 15, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
Shirmir D Branch, Amanda D French, Amanda M Lines, Brian M Rapko, William R Heineman, Samuel A Bryan
A protocol is presented that allows for the quantitative conversion and subsequent in situ spectroscopic analysis of [Re(CO)3]+ species in simulated Hanford tank waste. In this test case, the non-radioactive metal rhenium, is substituted for technetium (Tc-99), a weak beta emitter, to demonstrate proof of concept for a method to measure a non-pertechnetate form of technetium in Hanford tank waste. The protocol encompasses adding a simulated waste sample containing the non-emissive [Re(CO)3]+ species to a developer solution that enables the rapid, quantitative conversion of the non-emissive species to a luminescent species which can then be detected spectroscopically...
December 14, 2017: Environmental Science & Technology
Jan Philip Kraack, Laurent Sévery, S David Tilley, Peter Hamm
Intermolecular vibrational energy transfer in monolayers of isotopically mixed rhenium carbonyl complexes at solid-liquid interfaces is investigated with the help of ultrafast 2D Attenuated Total Reflectance Infrared (2D ATR IR) spectroscopy in dependence of plasmonic surface enhancement effects. Dielectric and plasmonic materials are used to demonstrate that plasmonic effects have no impact on the vibrational energy transfer rate in a regime of moderate IR surface enhancement (enhancement factors up to ca...
December 13, 2017: Journal of Physical Chemistry Letters
Aimin Ge, Benjamin Rudshteyn, Jingyi Zhu, Reinhard J Maurer, Victor S Batista, Tianquan Lian
A combination of time-resolved vibrational spectroscopy and density functional theory techniques have been applied to study the vibrational energy relaxation dynamics of the Re(4,4'-dicyano-2,2'-bipyridine)(CO)3Cl (Re(CO)3Cl) catalyst for CO2 to CO conversion bound to gold surfaces. The kinetics of vibrational relaxation exhibits a biexponential decay including an ultrafast initial relaxation and complete recovery of the ground vibrational state. Ab initio molecular dynamics simulations and time-dependent perturbation theory reveal the former to be due to vibrational population exchange between CO stretching modes and the latter to be a combination of intramolecular vibrational relaxation (IVR) and electron-hole pair (EHP) induced energy transfer into the gold substrate...
December 11, 2017: Journal of Physical Chemistry Letters
Samundeeswari Mariappan Balasekaran, Alfred P Sattelberger, Adelheid Hagenbach, Frederic Poineau
Quadruply bonded rhenium(III) dimers with the stoichiometry Re2L4F2 (1, L = hexahydro-2H-pyrimido[1,2a]pyrimidinate (hpp-); 2, L = diphenyl formamidinate (dpf-)) were prepared from the solid-state melt reactions (SSMRs) between (NH4)2[Re2F8]·2H2O and HL. Those compounds were characterized in the solid state by single-crystal X-ray diffraction and in solution by UV-visible spectroscopy and cyclic voltammetry. The compound [Re2(hpp)4F2]PF6 (3) was prepared from the one-electron oxidation of Re2(hpp)4F2 with [Cp2Fe]PF6...
December 8, 2017: Inorganic Chemistry
Yuanyuan Li, Qingfeng Liu, Qiannan Cui, Zeming Qi, Judy Z Wu, Hui Zhao
We report a comprehensive study on the effects of rhenium doping on optical properties and photocarrier dynamics of MoS2 monolayer, few-layer, and bulk samples. Monolayer and few-layer samples of Re-doped (0.6%) and undoped MoS2 were fabricated by mechanical exfoliation, and were studied by Raman spectroscopy, optical absorption, photoluminescence, and time-resolved differential reflection measurements. Similar Raman, absorption, and photoluminescence spectra were obtained from doped and undoped samples, indicating that the Re doping at this level does not significantly alter the lattice and electronic structures...
December 4, 2017: Nanoscale
Amr A A Attia, Alexandru Lupan, R Bruce King
Density functional theory studies on the rhenatricarbaboranes C3Bn-4Hn-1Re(CO)3 (n = 7-12) show that the lowest energy polyhedra for n-vertex metallaboranes having 2n + 2 skeletal electrons and sufficiently dissimilar vertex atoms can deviate from the most spherical closo deltahedra predicted by application of the Wade-Mingos rules. Furthermore, the lowest energy structures of these rhenatricarbaboranes are found to avoid C-C edges and have carbon atoms located at degree 4 rather than degree 5 vertices. The lowest energy structures for the 7-vertex C3B3H6Re(CO)3 system all have a central C3B3Re closo deltahedron, namely the pentagonal bipyramid with the rhenium atom at a degree 5 axial vertex and all three carbon atoms at degree 4 equatorial vertices...
November 29, 2017: Inorganic Chemistry
Shan-Shan Wang, Ying Liu, Zhi-Ming Yu, Xian-Lei Sheng, Shengyuan A Yang
Nonsymmorphic symmetries, which involve fractional lattice translations, can generate exotic types of fermionic excitations in crystalline materials. Here we propose a topological phase arising from nonsymmorphic symmetries-the hourglass Dirac chain metal, and predict its realization in the rhenium dioxide. We show that ReO2 features hourglass-type dispersion in the bulk electronic structure dictated by its nonsymmorphic space group. Due to time reversal and inversion symmetries, each band has an additional two-fold degeneracy, making the neck crossing-point of the hourglass four-fold degenerate...
November 29, 2017: Nature Communications
Allen J Osinski, Daniel L Morris, Richard S Herrick, Christopher J Ziegler
α-Amidinoazadi(benzopyrro)methenes were synthesized using the Re(CO)3 unit as a templating agent. The products of these template reactions are six-coordinate rhenium complexes, with a facial arrangement of carbonyls, a noncoordinating anion, and a tridentate α-amidinoazadi(benzopyrro)methene ligand. The tridentate ligand shows the conversion of one diiminoisoindoline sp2 carbon to a sp3 carbon, which has been seen in the "helmet" and bicyclic phthalocyanines. The bidentate diiminoisoindoline fragment tilts out of the plane of coordination...
November 27, 2017: Inorganic Chemistry
Fernando Barra, Artur Deditius, Martin Reich, Matt R Kilburn, Paul Guagliardo, Malcolm P Roberts
Rhenium and osmium isotopes have been used for decades to date the formation of molybdenite (MoS2), a common mineral in ore deposits and the world's main source of molybdenum and rhenium. Understanding the distribution of parent (187)Re and radiogenic daughter (187)Os isotopes in molybdenite is critical in interpreting isotopic measurements because it can compromise the accurate determination and interpretation of mineralization ages. In order to resolve the controls on the distribution of these elements, chemical and isotope mapping of MoS2 grains from representative porphyry copper-molybdenum deposits were performed using electron microprobe and nano-scale secondary ion mass spectrometry...
November 22, 2017: Scientific Reports
Delphine Séhédic, Igor Chourpa, Clément Tétaud, Audrey Griveau, Claire Loussouarn, Sylvie Avril, Claire Legendre, Nicolas Lepareur, Didier Wion, François Hindré, François Davodeau, Emmanuel Garcion
PURPOSE: Gold standard beam radiation for glioblastoma (GBM) treatment is challenged by resistance phenomena occurring in cellular populations well prepared to survive or to repair damage caused by radiation. Among signals that have been linked with radio-resistance, the SDF1/CXCR4 axis, associated with cancer stem-like cell, may be an opportune target. To avoid the problem of systemic toxicity and blood-brain barrier crossing, the relevance and efficacy of an original system of local brain internal radiation therapy combining a radiopharmaceutical with an immuno-nanoparticle was investigated...
2017: Theranostics
Nidal Saleh, Radovan Bast, Nicolas Vanthuyne, Christian Roussel, Trond Saue, Benoît Darquié, Jeanne Crassous
In our effort towards measuring the parity violation energy difference between two enantiomers, a simple chiral oxorhenium complex 5 bearing enantiopure 2-mercaptocyclohexan-1-ol has been prepared as a potential candidate species. Vibrational circular dichroism revealed a chiral environment surrounding the rhenium atom, even though the rhenium is not a stereogenic center itself, and enabled to assign the (1S,2S)-(-) and (1R,2R)-(+) absolute configuration for 5. For both compound 5 and complex 4, previously studied by us and bearing a propane-2-olato-3-thiolato ligand, relativistic calculations predict parity violating vibrational frequency differences of a few hundreds of millihertz, above the expected sensitivity attainable by a molecular beam Ramsey interferometer that we are constructing...
November 15, 2017: Chirality
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