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Dalton Transactions: An International Journal of Inorganic Chemistry

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https://www.readbyqxmd.com/read/28345728/embedding-1d-or-2d-cobalt-carboxylate-substrates-in-3d-coordination-polymers-exhibiting-slow-magnetic-relaxation-behaviors-crystal-structures-high-field-epr-and-magnetic-studies
#1
Nannan Mao, Biquan Zhang, Fan Yu, Xi Chen, Gui-Lin Zhuang, Zhenxing Wang, Zhongwen Ouyang, Tianle Zhang, Bao Li
By utilizing well-designed bifunctional ligands derived from 1H-imidazole-4,5-dicarboxylic acid, magnetic coordination polymers (CPs) that exhibit slow magnetic relaxation at the low temperature regions were constructed and further structurally characterized. In 1, 1D cobalt-carboxyl chains were stabilized in the final structure. In contrast, by adjusting the length of the substituted arms on imidazole-4,5-dicarboxylic acid, a novel 3D CP, 2 containing 2D 6(3) cobalt-carboxyl layer was obtained. A combination of Quantum Monte Carlo (QMC) simulations and the first-principles Density functional theory (DFT) calculations showed that compound 2 features weak ferro- and antiferro-magnetic coupling mechanisms with two different super-exchange paths of -/+/- for syn-anti carboxylate bridges and -/-/- for syn-syn carboxylate bridges...
March 27, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28345714/a-novel-symmetric-ttf-pyridyl-thiolato-zinc-complex-synthesis-characterization-and-crystal-structure-analysis
#2
Ryota Okuno, Minayo Yamaguchi, Hideki Fujiwara
We report the first preparation of a symmetric tetrathiafulvalene (TTF)-pyridyl thiolato zinc(ii) complex in which two TTF parts connect to the central zinc atom through pyridines and thiolates. We also discuss the crystal structure analysis and physical properties of the complex, especially photocurrent generations measured on its thin-film sample and single crystal.
March 27, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28345709/a-study-of-asymmetrical-mixed-valent-mo2-mo2-complexes-in-the-class-iii-regime
#3
Suman Mallick, Tao Cheng, Lu Chen, Miao Meng, Yu Yu Zhang, Chun Y Liu
Three novel asymmetrical dimolybdenum dimers, [Mo2(DAniF)3]2(μ-OOCCOS) (DAniF = N,N'-di(p-anisyl)formamidinate) ([OO-OS]), [Mo2(DAniF)3]2(μ-S2CCO2) ([SS-OO]), and [Mo2(DAniF)3]2(μ-SSCCOS) ([SS-OS]), have been synthesized and characterized by either single-crystal X-ray crystallography or (1)H NMR spectroscopy. The structural asymmetry for these compounds gives rise to a redox asymmetry, which enlarges the potential separation (ΔE1/2) between the two [Mo2] units. The mixed-valance (MV) species [OO-OS](+), [SS-OO](+) and [SS-OS](+), prepared by one-electron chemical oxidation of the neutral precursors, exhibit an intense and symmetrical intervalence charge transfer (IVCT) absorption band in the near-IR region, along with the high energy metal (δ) to ligand (π*) (ML) and ligand (π) to metal (δ) charge transfer (LMCT) absorptions...
March 27, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28345708/evaluation-of-two-and-three-dimensional-electrode-platforms-for-the-electrochemical-characterization-of-organometallic-catalysts-incorporated-in-non-conducting-metal-organic-frameworks
#4
Edgar Mijangos, Souvik Roy, Sonja Pullen, Reiner Lomoth, Sascha Ott
The development of a reliable platform for the electrochemical characterization of a redox-active molecular diiron complex, [FeFe], immobilized in a non-conducting metal organic framework (MOF), UiO-66, based on glassy-carbon electrodes is reported. Voltammetric data with appreciable current responses can be obtained by the use of multiwalled carbon nanotubes (MWCNT) or mesoporous carbon (CB) additives that function as conductive scaffolds to interface the MOF crystals in "three-dimensional" electrodes. In the investigated UiO-66-[FeFe] sample, the low abundance of [FeFe] in the MOF and the intrinsic insulating properties of UiO-66 prevent charge transport through the framework, and consequently, only [FeFe] units that are in direct physical contact with the electrode material are electrochemically addressable...
March 27, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28345707/selectivity-control-between-mizoroki-heck-and-homo-coupling-reactions-for-synthesising-multinuclear-metal-complexes-unique-addition-effects-of-tertiary-phosphines-and-o2
#5
Yasuomi Yamazaki, Osamu Ishitani
The addition of a tertiary phosphine and O2 to reaction solutions strongly affected the reactivity and selectivity of coupling reactions between transition metal complexes. The Mizoroki-Heck reaction between metal complexes with bromo and those with vinyl groups in the diimine ligand did not proceed using Pd(OAc)2 in the presence of 2-dicyclohexylphosphino-2',6'-dimethoxybiphenyl (Sphos) under Ar but proceeded selectively after injection of air into the reaction vessel. In the absence of the phosphine ligand, on the other hand, not only the Mizoroki-Heck reaction but also a homo-coupling reaction between the metal complexes with the bromo groups proceeded at the same time...
March 27, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28345706/topochemical-synthesis-of-cation-ordered-double-perovskite-oxynitrides
#6
Roberta Ceravola, Judith Oró-Solé, Ashley P Black, Clemens Ritter, Inés Puente Orench, Ignasi Mata, Elies Molins, Carlos Frontera, Amparo Fuertes
Topochemical nitridation in ammonia at moderate temperatures of cation ordered Sr2FeWO6 produces new antiferromagnetic double perovskite oxynitrides Sr2FeWO6-xNx with 0 < x ≤ 1. Nitrogen introduction induces the oxidation of Fe(2+) to Fe(3+) and decreases TN from 38 K (x = 0) to 13 K for Sr2FeWO5N which represents the first example of a double perovskite oxynitride with both high cationic order and nitrogen content. This synthetic approach can be extended to other cation combinations expanding the possibility of new materials in the large group of double perovskites...
March 27, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28345704/atomic-layer-deposition-of-nickel-cobalt-spinel-thin-films
#7
D J Hagen, T S Tripathi, M Karppinen
We report the atomic layer deposition (ALD) of high-quality crystalline thin films of the spinel-oxide system (Co1-xNix)3O4. These spinel oxides are ferrimagnetic p-type semiconductors, and promising material candidates for several applications ranging from photovoltaics and spintronics to thermoelectrics. The spinel phase is obtained for Ni contents exceeding the x = 0.33 limit for bulk samples. It is observed that the electrical resistivity decreases continuously with x while the magnetic moment increases up to x = 0...
March 27, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28345695/anion-dependent-self-assembly-of-copper-coordination-polymers-based-on-pyrazole-3-5-dicarboxylate-and-1-2-di-4-pyridyl-ethylene
#8
Fatima Klongdee, Jaursup Boonmak, Sujittra Youngme
By utilizing a pyrazole-3,5-dicarboxylic acid (H3pzdc) and flexible 1,2-di(4-pyridyl)ethylene (dpe) with various copper(ii) salts under the same solvothermal synthetic conditions, six novel coordination polymers, namely, {[Cu2(pzdc)(dpe)2]X}n (X = NO3(-) (1), ClO4(-) (2), BF4(-) (3), SCN(-) (4)), {[Cu(ii)4Cu(i)4(pzdc)4(dpe)6](H2O)4}2n (5), and {[Cu5(HPO4)2 (pzdc)2(dpe)3](H2O)5}n (6) were obtained. The structural diversity of compounds 1-6 depends on the starting Cu(ii) salts. Compounds 1-4 are isostructural and exhibit a 3D porous cationic pillar-layered coordination framework with lattice monoanions incorporated into the channels of the framework...
March 27, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28345088/near-infrared-emitting-iridium-iii-complexes-for-mitochondrial-imaging-in-living-cells
#9
Yuying Liu, Peipei Zhang, Xiaoqiang Fang, Gongqing Wu, Shuting Chen, Zhina Zhang, Hui Chao, Wenying Tan, Li Xu
Biocompatible transition metal complexes dyes emitting in the near-infrared (NIR) region, are highly desirable in fluorescence imaging techniques. However, a high-performance mitochondria-specific labeling NIR probe with high photostability is still lacking. Herein we reported two NIR-emitting cationic iridium(iii) complexes [Ir(pbq-g)2(N^N)](+)Cl(-) (pbq-g = phenylbenzo[g]-quinoline; N^N = 2-(1-benzyl-1H-pyrazol-3-yl) pyridine (Ir1) and 2-(1-(naphthalen-1-ylmethyl)-1H-pyrazol-3-yl) pyridine (Ir2)). These two novel Ir(iii) complexes with different N^N ligands exhibited similar NIR emission with λmax at 751 nm for Ir1 and 750 nm for Ir2 in PBS solution, with luminescence quantum yields of around 0...
March 27, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28345087/comment-on-conformational-analysis-of-triphenylphosphine-ligands-in-stereogenic-monometallic-complexes-tools-for-predicting-the-preferred-configuration-of-the-triphenylphosphine-rotor-by-j-f-costello-s-g-davies-e-t-f-gould-and-j-e-thomson-dalton-trans-2015
#10
LETTER
Henri Brunner, Takashi Tsuno
In half-sandwich compounds of the type [Cp*ML(1)L(2)PPh3] the PPh3 propeller is stabilized by attractive CH/π interactions in which Co-H bonds specifically interact with the Ci and Co atoms of neighbouring phenyl rings, as in the T-shaped benzene dimer (i/o = ipso/ortho). This stabilization was not taken into account in a recent conformational analysis based on van der Waals energy calculations and minimization of steric compression (Dalton Trans., 2015, 44, 5451-5466). It is shown that in all 116 structures discussed in this analysis the CoH-Ci/o distances fall below the sum of the van der Waals radii, establishing attractive CH/π interactions, although the short contacts could easily be avoided by phenyl rotation to relieve steric strain...
March 27, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28345086/selective-c-c-coupling-at-a-pt-iv-centre-100-preference-for-sp-2-sp-3-over-sp-3-sp-3
#11
Paul A Shaw, Jonathan P Rourke
The oxidative addition of three different organic halides RX to the non-symmetric platinum(ii) mer coordinated dicyclometallated C^N^C complex 1 yielded short-lived six-coordinate platinum(iv) complexes 2(R) (R = Me, allyl, Bn), with the incoming groups trans across the platinum centre. A spontaneous reductive coupling reaction then occurred with, in each case, a completely chemoselective sp(2)-sp(3) coupling, and exclusively gave R-3, with the newly introduced R group bonded to the previously cyclometallated aryl ring...
March 27, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28338141/structurally-related-hydrazone-based-metal-complexes-with-different-antitumor-activities-variably-induce-apoptotic-cell-death
#12
Dominik A Megger, Kristin Rosowski, Christian Radunsky, Jutta Kösters, Barbara Sitek, Jens Müller
Three new complexes bearing the tridentate hydrazone-based ligand 2-(2-(1-(pyridin-2-yl)ethylidene)hydrazinyl)pyridine (L) were synthesized and structurally characterized. Biological tests indicate that the Zn(ii) complex [ZnCl2(L)] is of low cytotoxicity against the hepatocellular carcinoma cell line HepG2. In contrast, the Cu(ii) and Mn(ii) complexes [CuCl2(L)] and [MnCl2(L)] are highly cytotoxic with EC50 values of 1.25 ± 0.01 μM and 20 ± 1 μM, respectively. A quantitative proteome analysis reveals that treatment of the cells with the Cu(ii) complex leads to a significantly altered abundance of 102 apoptosis-related proteins, whereas 38 proteins were up- or down-regulated by the Mn(ii) complex...
March 24, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28338136/investigation-of-the-complexation-of-nat-zr-iv-and-89-zr-iv-by-hydroxypyridinones-for-the-development-of-chelators-for-pet-imaging-applications
#13
F Guérard, M Beyler, Y-S Lee, R Tripier, J-F Gestin, M W Brechbiel
Three hydroxypyridinone (HOPO) positional isomers - 1,2-HOPO (L1H) and its water soluble analogue (L1'H), 3,2-HOPO (L2H) and 3,4-HOPO (L3H) have been investigated for the complexation of Zr(iv). Potentiometric and UV-Vis spectrometric studies show a higher thermodynamic stability for the formation of Zr(L1')4 in comparison with Zr(L2)4 and Zr(L3)4 as well as a higher kinetic inertness in competition studies with EDTA or Fe(3+) at a radiotracer concentration with (89)Zr. Besides the low pKa of L1H or L1'H (pKa = 5...
March 24, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28332684/dft-calculations-as-a-ligand-toolbox-for-the-synthesis-of-active-initiators-for-rop-of-cyclic-esters
#14
D Jędrzkiewicz, D Kantorska, J Wojtaszak, J Ejfler, S Szafert
New heteroleptic zinc dimeric complexes bearing an aminophenolate ligand of a single-site initiator framework were synthesized and characterized by spectroscopic methods, X-ray analysis, and DFT calculations. The theoretical study, verified by the experimental data, explains the catalytic behaviour in the ROP of lactide in the examined zinc complexes. The presented simple DFT protocol constitutes a valuable method for the qualification of the ancillary ligand to rationally design new complexes to improve their catalytic activity...
March 23, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28332683/tailoring-adsorption-induced-phase-transitions-in-the-pillared-layer-type-metal-organic-framework-dut-8-ni
#15
Negar Kavoosi, Volodymyr Bon, Irena Senkovska, Simon Krause, Cesare Atzori, Francesca Bonino, Julia Pallmann, Silvia Paasch, Eike Brunner, Stefan Kaskel
Tailoring the characteristics of gating transitions in the porous network, Ni2(ndc)2dabco (ndc = 2,6-naphthalenedicarboxylate, dabco = 1,4-diazabicyclo[2.2.2]octane), also termed DUT-8(Ni) (DUT = Dresden University of Technology), was achieved by systematically adjusting the critical synthesis parameters. The impact of the starting composition and solvent mixtures in the synthesis was found to critically affect the guest-response properties of the obtained materials. A comprehensive set of physical characterization methods, namely thermal analysis, (1)H NMR of digested crystals, solid state (13)C NMR, PXRD, SEM, IR and Raman spectroscopy shows that the crystallite size is a crucial factor, determining the differing characteristics such as "gate pressure" and adsorption capacity in the guest-responsive switching behaviour of DUT-8...
March 23, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28332680/templated-and-template-free-fabrication-strategies-for-zero-dimensional-hollow-mof-superstructures
#16
Hyehyun Kim, Myoung Soo Lah
Various fabrication strategies for hollow metal-organic framework (MOF) superstructures are reviewed and classified using various types of external templates and their properties. Hollow MOF superstructures have also been prepared without external templates, wherein unstable intermediates obtained during reactions convert to the final hollow MOF superstructures. Many hollow MOF superstructures have been fabricated using hard templates. After the core-shell core@MOF structure was prepared using a hard template, the core was selectively etched to generate a hollow MOF superstructure...
March 23, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28332677/tuneable-reversible-redox-of-cobalt-iii-carbazole-complexes
#17
Michael S Bennington, Humphrey L C Feltham, Zoë J Buxton, Nicholas G White, Sally Brooker
Four tridentate carbazole-based ligands, HL((t)Bu/H) {3,6-di(tert-butyl)-1,8-bis[5-(3-benzyl-1,2,3-triazole)]-9H-carbazole}, HL((t)Bu/(t)Bu) {3,6-di(tert-butyl)-1,8-bis[5-(3-(4-tert-butyl)benzyl-1,2,3-triazole)]-9H-carbazole}, HL(H/H) {1,8-bis[5-(3-benzyl-1,2,3-triazole)]-9H-carbazole} and HL(H/(t)Bu) {1,8-bis[5-(3-(4-tert-butyl)benzyl-1,2,3-triazole)]-9H-carbazole}, were prepared and complexed with cobalt(ii) tetrafluoroborate. In situ air oxidation resulted in cobalt(iii) complexes 1-4 with the general formula [Co(III)(L)2]BF4·xH2O (1: L = L((t)Bu/H), x = 2; 2: L = L((t)Bu/(t)Bu), x = 1; 3: L = L(H/H), x = 0...
March 23, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28332676/application-of-the-dimensional-reduction-formalism-to-pb9-xbax-li2-p2o7-2-p4o13-2-x-0-2-6-7-a-series-of-phosphates-with-two-types-of-isolated-polyphosphate-groups
#18
Xiangyu Zhang, Hongping Wu, Qiong Liu, Xiaoyu Dong, Yunlei Chen, Zhihua Yang, Xiao-Dong Wen, Shilie Pan
A series of phosphates, Pb9-xBax[Li2(P2O7)2(P4O13)2] (x = 0, 2, 6, 7), have been synthesized by a high temperature solution method and the crystal structures were determined by single crystal X-ray diffraction. They are isostructural and crystallize in the triclinic space group P1[combining macron]. It is interesting that there are two kinds of isolated polyphosphate anionic groups coexisting in the crystal structure, which is rare among phosphates. Their structures exhibit zero-dimensional [Li2(P2O7)2(P4O13)2](18-) anionic clusters constructed by the LiO4, P2O7 and P4O13 groups, which are separated by the Pb(2+) or Ba(2+) cations...
March 23, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28332673/hierarchical-porous-nico2o4-nanosheet-arrays-directly-grown-on-carbon-cloth-with-superior-lithium-storage-performance
#19
Li Zhao, Lei Wang, Peng Yu, Chungui Tian, He Feng, Zhongwei Diao, Honggang Fu
Binary metal oxides have been explored as advanced candidates in lithium-ion battery (LIB) anodes due to their high specific capacity. Herein, the hierarchical structures of porous NiCo2O4 nanosheets directly grown on a conductive carbon cloth substrate (3D NCO-PSA/CC) were obtained by a facile in situ synthetic strategy. When applied as a binder-free LIB anode, it exhibited satisfactory performance with a high discharge capacity (a first discharge capacity of 2090.8 mA h g(-1) and a stable capacity of 1687...
March 23, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28332672/formation-of-paramagnetic-metallacyclobutadienes-by-reaction-of-diaminoacetylenes-with-molybdenum-alkylidyne-complexes
#20
Òscar Àrias, Kai Brandhorst, Dirk Baabe, Matthias Freytag, Peter G Jones, Matthias Tamm
The reactions of the molybdenum alkylidyne complex [MesC[triple bond, length as m-dash]Mo{OCMe(CF3)2}3] (1) with the diaminoacetylenes R2NC[triple bond, length as m-dash]CNR2 (2, NR2 = 4-methylpiperidinyl; 3, NR2 = NEt2; Mes = 2,4,6-trimethylphenyl) afforded the metallacyclobutadiene (MCBD) complexes 4 and 5. In contrast to all other MCBD complexes, 4 and 5 are paramagnetic and best described as Mo(iv) species containing an anionic diaminodicarbene of the type [(R2N)CC(Mes)C(NR2)](-).
March 23, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
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