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Dalton Transactions: An International Journal of Inorganic Chemistry

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https://www.readbyqxmd.com/read/28524924/a-theoretical-study-on-the-mechanistic-highlights-behind-the-br%C3%A3-nsted-acid-dependent-mer-fac-isomerization-of-homoleptic-carbenic-iridium-complexes-for-pholeds
#1
Tobias Setzer, Christian Lennartz, Andreas Dreuw
Recently, a successful Brønsted-acid mediated geometric isomerization of the meridional homoleptic carbenic iridium(iii) complexes tris-(N-phenyl,N-methyl-benzimidazol-2-yl)iridium(iii) (1) and tris-(N-phenyl,N-benzyl-benzimidazol-2-yl)iridium(iii) (2) into their facial form has been reported. In the present work the pronounced acid-dependency of this particular isomerization procedure is revisited and additional mechanistic pathways are taken into account. Moreover, the acid-induced material decomposition is addressed...
May 19, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28524209/understanding-the-biomimetic-properties-of-gallium-in-pseudomonas-aeruginosa-an-xas-and-xps-study
#2
F Porcaro, C Bonchi, A Ugolini, E Frangipani, G Polzonetti, P Visca, C Meneghini, C Battocchio
Pyochelin (PCH) is a siderophore (extracellular chelator) produced by the pathogenic bacterium Pseudomonas aeruginosa (PAO). PCH is implicated in iron (Fe(3+)) transport to PAO, and is crucial for its metabolism and pathogenicity. Due to the chemical similarity with Fe(3+), gallium (Ga(3+)) interferes with vital iron-dependent processes in bacterial cells, thereby opening new perspectives for the design of specific metal-based antibacterial drugs. However, the structural basis for the Fe(3+)-mimetic properties of Ga(3+) complexed with the PCH siderophore is still lacking...
May 19, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28524205/structure-and-luminescence-analyses-of-simultaneously-synthesised-lu1-xgdx-2o2s-tb-3-and-lu1-xgdx-2o3-tb-3
#3
Natalie Pasberg, Daniel den Engelsen, George R Fern, Paul G Harris, Terry G Ireland, Jack Silver
Herein we describe the synthesis and luminescence of nanosized (Lu1-y-xGdx)2O2S:Tby and (Lu1-y-xGdx)2O3:Tby phosphors with y = 0.1 mol% Tb(3+) and y = 2 mol% Tb(3+) and x ranging between 0 and 1. The concentration of Gd(3+) (x) was varied in steps of 0.1 (molar ratio Gd(3+)). The samples at 0.1 < x < 0.7 contained a mixture of (Lu1-xGdx)2O3:Tb(3+) and (Lu1-xGdx)2O2S:Tb(3+), while the samples at x = 0 contained only Lu2O3:Tb(3+). At 0.1 < x < 0.7 Lu2O2S:Tb(3+) and Gd2O2S:Tb(3+) did not form a solid solution, but rather crystallised into two slightly different hexagonal structures...
May 19, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28524197/a-cuboidal-ni4o4-cluster-as-a-precursor-for-recyclable-carbon-supported-nickel-nanoparticle-reduction-catalysts
#4
Yan-Qiu Yuan, Feng-Ling Yuan, Fei-Long Li, Zhi-Min Hao, Jun Guo, David J Young, Wen-Hua Zhang, Jian-Ping Lang
Cuboidal [Ni4O4] clusters supported by a pyridine alkoxide ligand have been developed. One of these clusters was selected as a precursor for carbon-hosted Ni nanoparticles (NiNPs/C) which were efficient catalysts for the conversion of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) at room temperature.
May 19, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28518206/organocatalytic-hydroborylation-promoted-by-n-heterocyclic-olefins
#5
Christian Hering-Junghans, Ian C Watson, Michael J Ferguson, Robert McDonald, Eric Rivard
New complexes containing N-heterocyclic vinylene-stabilized [B2H5](+) fragments were prepared, and surprisingly it was found that the precursor N-heterocyclic olefins (NHOs) could promote the mild (room temperature) catalytic hydroborylation of ketones and aldehydes. This finding represents an important addition to the burgeoning field of non-metal mediated catalysis.
May 18, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28518202/improved-reactivity-of-a-cyclic-13-15-compound-by-increased-steric-demand
#6
Markus Balmer, Manuel Kapitein, Carsten von Hänisch
Herein we present the synthesis and characterization of the new four-membered Ga/P cycle [tBu2GaP(H)SitBu2Ph]2, which shows a cis/trans isomerization at ambient temperatures via a ring opening mechanism. The sterically demanding substituents on the phosphorus (-SitBu2Ph) and gallium (tBu) atoms lead to an unexpected reactivity towards bulky NHC ligands (IMes and IDipp). The resulting Lewis base stabilized monomeric 13/15 compounds feature an unusual binding mode of the carbene ligand. The ring opened state also enables a masked flp reactivity, which is shown by a reaction with the polar multiple bond in Ph-NCO...
May 18, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28518191/latio2n-lacro3-continuous-solid-solutions-towards-enhanced-photocatalytic-h2-evolution-under-visible-light-irradiation
#7
Jinwen Shi, Yazhou Zhang, Zhaohui Zhou, Yixiang Zhao, Jingyuan Liu, Hongbing Liu, Xiang Liao, Yuchao Hu, Daming Zhao, Shaohua Shen
(LaTiO2N)1-x(LaCrO3)x continuous solid solutions with an orthorhombic-phase ABX3 perovskite structure and with varied LaCrO3 contents (0 ≤ x ≤ 1) were synthesized by a polymerized complex method followed by a post-treatment process of nitridation for the first time. Visible-light-driven photocatalytic H2-evolution activities of the solid solutions gradually increased with the increase of x from 0.0 to 0.3, and then sharply decreased with the further increase of x from 0.3 to 1.0. With the increase of x, on the one hand, the narrowed bandgaps of solid solutions would enhance the generation of charge carriers and the increased lattice distortion of solid solutions could promote the separation and migration of charge carriers, thus mainly contributing to the improvement of photocatalytic activities; on the other hand, the lowered CBMs of solid solutions would reduce the driving force for reducing H2O to H2 and the decreased surface areas of solid solutions would weaken the adsorption of reactants and reduce the reactive sites, thereby resulting in the deterioration of photocatalytic activities...
May 18, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28518190/sequential-incorporation-of-metallic-cations-cd-2-and-hg-2-and-n-octylamine-into-titanium-phosphate-nanoparticles-and-their-subsequent-release-in-acid-media
#8
Javier Carrasco-Rodríguez, Daniel Martín-Yerga, Leoncio Garrido, Agustín Costa-García, Francisco J García Alonso
Titanium phosphate nanoparticles, TPNP, consisting of a NaTi2(PO4)3 core and a shell of hydrogen phosphate and dihydrogen phosphate of titanium, undergo fast hydrolysis in water releasing phosphoric acid. This reaction is inhibited in the presence of metallic ions like Cd(2+) or Hg(2+), which are able to replace the protons of the shell acid phosphates. The amount of the adsorbed metallic cations could be regulated using counterions of different basicity. The resulting nanoparticles also incorporate NH2(CH2)7CH3 (N-octylamine) at room temperature forming N-octylammonium/phosphate ion pairs, but it was found that at higher cation concentration inside the nanoparticle, a lower amount of amine was adsorbed...
May 18, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28517014/n-atom-transfer-via-thermal-or-photolytic-activation-of-a-co-azido-complex-with-a-pnp-pincer-ligand
#9
V Vreeken, L Baij, B de Bruin, M A Siegler, J I van der Vlugt
Thermal or photolytic activation of well-defined mononuclear [Co(N3)(PNP)] (PNP = 2,2'-bis(diisopropylphosphino)-4,4'-ditolylamido) results in the structurally characterized dinuclear species [Co(μ-N;κ(3)-P,N,N-PN(P)N)]2 (3), with two N-bridging phosphiniminato bridgeheads. Density Functional Theory (DFT) calculations indicate the intermediacy of a mononuclear cobalt-nitrido complex, followed by N-migratory insertion into a Co-P bond. Reaction of 3 with two equiv. HCl leads to rupture of the dimer with formation of mononuclear [CoCl(PN(P)N(H))] (4) by protonation of the N-bridges...
May 18, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28517006/synthesis-and-characterization-of-a-family-of-thioether-dithiolate-bridged-heteronuclear-iron-complexes
#10
Yahui Zhang, Dawei Yang, Ying Li, Baomin Wang, Xiangyu Zhao, Jingping Qu
The thioether-dithiolate-bridged heterotrinuclear complexes [Cp*Fe(μ-1k(3)SSS':2k(2)SS-tpdt)M(μ-2k(2)SS:3k(3)SSS'-tpdt)FeCp*][PF6]2 (Cp* = η(5)-C5Me5; tpdt = S(CH2CH2S)2; 2, M = Co; 3, M = Ni; 4, M = Pd) have been prepared by a reaction of [Cp*Fe(η(3)-tpdt)] (1) with complexes CoCl2, NiCl2(PPh3)2, and PdCl2(PPh3)2, respectively. Similarly, treatment of complex 1 with CuCl(PPh3) or AgPF6 afforded two heterotrinuclear complexes, [Cp*Fe(μ-1k(3)SSS':2k(2)SS-tpdt)M(μ-2k(2)SS:3k(3)SSS'-tpdt)FeCp*][PF6] (5, M = Cu; 6, M = Ag), while reaction of 1 with the complex AuCl(PPh3) gave a heterobinuclear complex, [Cp*Fe(μ-1k(3)SSS':2k(1)S-tpdt)Au(PPh3)][PF6] (7)...
May 18, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28517002/modulation-of-the-fe-ii-spin-crossover-effect-in-the-pentadecanuclear-fe9-m-cn-8-6-m-re-w-clusters-by-facial-coordination-of-tridentate-polyamine-ligands
#11
Szymon Chorazy, Jan J Stanek, Jedrzej Kobylarczyk, Shin-Ichi Ohkoshi, Barbara Sieklucka, Robert Podgajny
Spin crossover (SCO) materials, revealing the externally tunable transition between two different spin states, arouse great scientific interest due to their perspective application in information storage, display devices and sensing. Of special importance are the molecular systems offering the possibility of multimodal switching within many spin centers. This is achievable in polynuclear clusters consisting of several SCO-active complexes, however, such molecules are very rare. Herein, we report a unique pair of nanometric pentadecanuclear {Fe9[M(CN)8]6(Me3tacn)8}·14MeOH (Me3tacn = 1,4,7-trimethyl-1,4,7-triazacyclononane, M = Re, 1; M = W, 2) clusters exhibiting a thermally induced spin crossover effect on Fe(ii) complexes, that is on both central and external Fe sites embedded in the cyanido-bridged cluster core...
May 18, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28516992/a-nano-silver-xerogel-ag-nps-modified-teos-as-a-newly-developed-nanocatalyst-in-the-synthesis-of-benzopyranopyrimidines-with-secondary-and-primary-amines-and-gem-bisamides
#12
Gurpreet Kour, Monika Gupta
Silver nanoparticles have been prepared from a chemical reduction approach and supported on modified TEOS (tetraethylorthosilicate) xerogels to be studied as a nanocatalyst in the conversions of benzopyranopyrimidines (with primary as well as secondary amines along with the mechanism by trapping the imine intermediate) and also in the synthesis of gem-bisamides. Different conditions for the performance of the nanocatalyst have been screened and tolerance with respect to variable functionalities has been observed, resulting in excellent yields; and confirmation of products synthesized has been done using studies like (1)H NMR, (13)C NMR and mass analysis...
May 18, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28516988/syntheses-and-catalytic-oxotransfer-activities-of-oxo-molybdenum-vi-complexes-of-a-new-aminoalcohol-phenolate-ligand
#13
M K Hossain, M Haukka, R Sillanpää, D A Hrovat, M G Richmond, E Nordlander, A Lehtonen
The new aminoalcohol phenol 2,4-di-tert-butyl-6-(((2-hydroxy-2-phenylethyl)amino)methyl)phenol (H2L) was prepared by a facile solvent-free synthesis and used as a tridentate ligand for new cis-dioxomolybdenum(vi)(L) complexes. In the presence of a coordinating solvent (DMSO, MeOH, pyridine), the complexes crystallise as monomeric solvent adducts while in the absence of such molecules, a trimer with asymmetric Mo[double bond, length as m-dash]O→Mo bridges crystallises. The complexes can catalyse epoxidation of cis-cyclooctene and sulfoxidation of methyl-p-tolylsulfide, using tert-butyl hydroperoxide as oxidant...
May 18, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28513747/structural-and-electronic-elucidation-of-a-n-heterocyclic-silylene-vanadocene-adduct
#14
Mikko M Hänninen, Amgalanbaatar Baldansuren, Thomas Pugh
The solid and solution state structure of the vanadium(ii) N-heterocyclic silylene (NHSi) complex, [((Si)IPr)V(Cp)2] (1) is reported ((Si)IPr: 1,3-bis(2,6-diisopropylphenyl)-1,3-diaza-2-silacyclopent-4-en-2-ylidene). The electronic structure of 1 is probed using a combination of magnetic measurements, EPR spectroscopy and computational studies. The V-Si bond strength and complex forming mechanism between vanadocene and an NHSi ligand is elucidated using computational methods.
May 17, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28513741/magneto-structural-correlations-in-a-family-of-di-alkoxo-bridged-chromium-dimers
#15
Hector W L Fraser, Gary S Nichol, Gunasekaran Velmurugan, Gopalan Rajaraman, Euan K Brechin
A series of di-alkoxo bridged Cr(iii) dimers have been synthesised using pyridine alcohol ligands. The structures fall into four general categories and are of formula: [Cr2(OMe)2(pic)4]·½MeOH·½Et2O (1), [Cr2(hmp)2(pic)2X2] (where X = Cl (2), Br (3)), [Cr2(L)2Cl4(A)2]·2S (where L = hmp, A = H2O and S = Et2O (4); L = hmp, A = pyridine and S = pyridine (5); L = hmp, A = 4-picoline and no S (6); L = hep, A = H2O and S = MeCN (7)), and [Cr(hmp)(hmpH)Cl2]·MeCN (8). Direct current (DC) magnetic susceptibility measurements show relatively weak antiferromagnetic exchange interactions between the Cr(iii) centres with J values <|15| cm(-1) in all of the complexes measured...
May 17, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28513731/ag-au-nanoprism-metal-organic-framework-based-paper-for-extending-the-glucose-sensing-range-in-human-serum-and-urine
#16
Pin-Hsuan Huang, Chia Ping Hong, Jian Fan Zhu, Tzu-Ting Chen, Chu-Ting Chan, Yu-Chien Ko, Tien-Li Lin, Zheng-Bang Pan, Ning-Kuei Sun, Ying-Chu Wang, Jong-Jheng Luo, Tzu-Chieh Lin, Chia-Cheng Kang, Jing-Jong Shyue, Mei-Lin Ho
In this work, we present a Ag@Au nanoprism-metal-organic framework-paper based glucose sensor for rapid, sensitive, single-use and quantitative glucose determination in human serum. To achieve painless measurement of glucose with a non-invasive detection methodology, this biosensor was further tested in human urine. In this approach, a new hybrid-Ag@Au nanoprism loaded in close proximity to micrometer sized coordination polymers as phosphorescent luminophores significantly enhanced the emission intensity due to metal-enhanced phosphorescence and worked as reaction sites to support more dissolved oxygen...
May 17, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28513726/delocalized-and-localized-donating-accepting-mn-c-interactions-in-half-sandwich-cyclopentadienyl-and-pentadienyl-complexes
#17
Josué Solís-Huitrón, Noé Zúñiga-Villarreal, Diego Martínez-Otero, José Enrique Barquera-Lozada
The widely used cyclopentadienyl (Cp) ligand and the pentadienyl (Pdl) ligand have very similar molecular orbitals (MOs) but they have significantly different chemical behavior. The extensively mixing of the MOs in the Pdl ligand has prevented a quantitative explanation of the observed differences between these two ligands. In a series of synthesized close/open half sandwich manganese phosphine carbonyls, the quantum theory of atoms in molecules and the interacting quantum atom model allow us to quantify the accepting-donating capacities of both ligands and to break down the M-dienyl bond into individual atomic interactions...
May 17, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28513723/amphiphilic-coatings-for-the-protection-of-upconverting-nanoparticles-against-dissolution-in-aqueous-media
#18
Olivija Plohl, Slavko Kralj, Boris Majaron, Eleonore Fröhlich, Maja Ponikvar-Svet, Darko Makovec, Darja Lisjak
Upconverting nanoparticles (UCNPs) of β-NaYF4, co-doped with Yb(3+) and Tm(3+) and 21-36 nm large, were synthesized using a modified thermal decomposition method. The as-synthesized UCNPs were coated with oleic acid and dispersed in nonpolar media. Their morphology, size and crystal structure were analysed with transmission electron microscopy and X-ray diffraction. The UCNPs showed a fluorescence emission spectrum characteristic of Tm(3+). Their dissolution in water (pH ∼ 4-5) and phosphate buffered saline (PBS, pH = 7...
May 17, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28513693/synthesis-characterization-and-in-vitro-and-in-vivo-anticancer-activity-of-pt-iv-derivatives-of-pt-1s-2s-dach-5-6-dimethyl-1-10-phenanthroline
#19
Benjamin W J Harper, Emanuele Petruzzella, Roman Sirota, Fernanda Fabiola Faccioli, Janice R Aldrich-Wright, Valentina Gandin, Dan Gibson
This report describes the synthesis, characterization and biological activity of a series of platinum(iv) derivatives of [Pt(1S,2S-DACH)(5,6-dimethyl-1,10-phenanthroline)] (Pt56MeSS) with non-bioactive, lipophilic and bioactive axial ligands. In an attempt to explore the anticancer activity potential of the Pt(iv) derivatives, 2D and 3D cytotoxic screening and a preliminary in vivo study were performed. The average IC50 values of the platinum(iv) derivatives ranged from 1.26 to 5.39 μM, compared with 1.24 μM for Pt56MeSS, suggesting that the axial ligands have a relatively minor effect on the potency of the compounds...
May 17, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28513689/proton-conduction-in-a-hydrogen-bonded-complex-of-copper-ii-bipyridine-glycoluril-nitrate
#20
Sakharam B Tayade, Vishal M Dhavale, Avinash S Kumbhar, Sreekumar Kurungot, Peter Lönnecke, Evamarie Hey-Hawkins, Bhalchandra Pujari
Bipyridine glycoluril (BPG), a urea-fused bipyridine tecton, forms a square-pyramidal secondary building unit with copper(ii) which further self-assembles to give a porous hydrogen-bonded complex. This complex displays a high proton conductivity of 4.45 × 10(-3) S cm(-1) at 90 °C and 95% relative humidity (RH). Chains consisting of coordinated water, solvent water and nitrate anions embedded in the complex are responsible for high proton conduction. The proton conduction pathway was corroborated by ab initio electronic structure calculations with molecular dynamics (MD) simulations using the Nudged Elastic Band (NEB) method...
May 17, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
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