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Dalton Transactions: An International Journal of Inorganic Chemistry

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https://www.readbyqxmd.com/read/30020281/impact-of-the-lanthanide-contraction-on-the-activity-of-a-lanthanide-dependent-methanol-dehydrogenase-a-kinetic-and-dft-study
#1
Henning Lumpe, Arjan Pol, Huub J M Op den Camp, Lena J Daumann
Interest in the bioinorganic chemistry of lanthanides is growing rapidly as more and more lanthanide-dependent bacteria are being discovered. Especially the earlier lanthanides have been shown to be preferentially utilized by bacteria that need these Lewis acids as cofactors in their alcohol dehydrogenase enzymes. Here, we investigate the impact of the lanthanide ions lanthanum(iii) to lutetium(iii) (excluding Pm) on the catalytic parameters (vmax, KM, kcat/KM) of a methanol dehydrogenase (MDH) isolated from Methylacidiphilum fumariolicum SolV...
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30020278/synthesis-of-glycerol-carbonate-over-a-2d-coordination-polymer-built-with-nd-3-ions-and-organic-ligands
#2
Chris H J Franco, Poliane Chagas, Gabriela S Caldeira, Luiz C A Oliveira, Patterson P de Souza, Alexandre A Leitão, Giovanni W Amarante, Renata Diniz
In this work, a two-dimensional coordination polymer was synthesized and the structure was determined by single-crystal X-ray diffraction. The crystal structure belongs to the space group Pna21 and was characterized by Raman and FT-infrared spectroscopy, powder X-ray diffraction and Brunauer-Emmett-Teller surface area analysis. Catalyst activities were evaluated through the synthesis of glycerol carbonate from glycerol and urea using a batch reactor. After the optimization of both reaction and reaction conditions, the activity results showed that the coordination polymer used as a heterogeneous catalyst has good values of conversions and selectivity for the manufacturing of glycerol carbonate in a fine-chemical process...
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30019733/heterometallic-cu-ii-fe-iii-and-cu-ii-mn-iii-alkoxo-bridged-complexes-revealing-a-rare-hexanuclear-m-6-%C3%AE-x-7-%C3%AE-3-x-2-molecular-core
#3
Oksana V Nesterova, Dmytro S Nesterov, Beáta Vranovičová, Roman Boča, Armando J L Pombeiro
The novel hexanuclear complexes [Cu4Fe2(OH)(Piv)4(tBuDea)4Cl]·0.5CH3CN (1) and [Cu4Mn2(OH)(Piv)4(tBuDea)4Cl] (2) were prepared through one-pot self-assembly reactions of copper powder and iron(ii) or manganese(ii) chloride with N-tert-butyldiethanolamine (H2tBuDea) and pivalic acid (HPiv) in acetonitrile. Crystallographic studies revealed the uncommon molecular core type M6(μ-X)7(μ3-X)2 in 1 and 2, which can be viewed as a combination of two trimetallic M3(μ-X)2(μ3-X) fragments joined by three bridging atoms...
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30019732/a-cu-ii-metallocycle-for-the-reversible-self-assembly-of-coordination-driven-polyrotaxane-like-architectures
#4
Giada Truccolo, Zeno Tessari, Jacopo Tessarolo, Silvio Quici, Lidia Armelao, Marzio Rancan
We report the design and synthesis of a Cu(ii) metallocycle (1) and use the possibility to expand the Cu(ii) coordination sphere to self-assemble mechanically interlocked species via interpenetration. Metallocycle 1 can be used as a platform to reversibly assemble a 1D + 1D → 1D coordination-driven polyrotaxane (3), where 1 acts as the hosting ring as well as the stopper, and 4,4'-bipyridine is the guest-axle. A coordinating solvent can substitute the 4,4'-bipyridine axle to disassemble the polyrotaxane (3 → 2) that is easily restored by further adding 4,4'-bipyridine (2 → 3)...
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30019730/bivo-4-quantum-dot-decorated-bipo-4-nanorods-0d-1d-heterojunction-for-enhanced-visible-light-driven-photocatalysis
#5
Boyuan Li, Zhenhua Cao, Shixuan Wang, Qiang Wei, Zhurui Shen
Herein, we report a BiVO4 quantum dot (QDs)-decorated BiPO4 nanorods 0D/1D heterojunction via an in situ growth method. It showed enhanced visible-light-driven photocatalytic activity for degrading Rhodamine B (Rh B) compared to its pristine counterparts in composite. The mass ratio of BiVO4/BiPO4 was then varied from 3 wt% to 50 wt% and the optimum value was found to be 30 wt%, showing 8.3-fold and 6.3-fold apparent reaction rates higher than those of pristine BiPO4 and BiVO4, respectively. Moreover, all of the reduced Rh B was transformed into CO2 and H2O during the photocatalysis, thus showing the good mineralization ability (almost 100%) of the composite...
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30019727/covalently-linking-cuins-2-quantum-dots-with-a-re-catalyst-by-click-reaction-for-photocatalytic-co-2-reduction
#6
Jing Huang, Mélina Gilbert Gatty, Bo Xu, Palas Baran Pati, Ahmed S Etman, Lei Tian, Junliang Sun, Leif Hammarström, Haining Tian
Covalently linking photosensitizers and catalysts in an inorganic-organic hybrid photocatalytic system is beneficial for efficient electron transfer between these components. However, general and straightforward methods to covalently attach molecular catalysts on the surface of inorganic semiconductors are rare. In this work, a classic rhenium bipyridine complex (Re catalyst) has been successfully covalently linked to the low toxicity CuInS2 quantum dots (QDs) by click reaction for photocatalytic CO2 reduction...
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30019726/oxidatively-stable-ferrocenyl-%C3%AF-bridge-titanocene-d-%C3%AF-a-complexes-an-electrochemical-and-spectroscopic-investigation-of-the-mixed-valent-states
#7
Jared A Pienkos, Alexander B Webster, Eric J Piechota, A Danai Agakidou, Colin D McMillen, David Y Pritchett, Gerald J Meyer, Paul S Wagenknecht
The synthesis, spectroscopic, and electrochemical characterization of oxidatively stable D-π-A compounds of the form (Me2CpC2Fc)2TiCl2 and RCp2Ti(C2Fc)2CuX (where Fc = ferrocenyl) are reported. Oxidative stability enabled by the addition of CuX is evidenced by voltammagrams of the RCp2Ti(C2Fc)2CuX compounds which all display two chemically-reversible 1e- FeIII/II couples, indicative of electronic communication between the Fc- termini. Differential pulse voltammetry (DPV) in CH2Cl2/[n-Bu4N][PF6], demonstrated that the redox potential difference between the two 1e- FeIII/II couples (ΔE1/2) is between 112 mV and 146 mV, being most pronounced with the electron rich Cp*2Ti(C2Fc)2CuBr...
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30019725/stabilizing-intramolecular-cobalt-imidazole-coordination-with-a-remote-methyl-group-in-the-backbone-of-a-cofactor-b-12-protein-model
#8
Marjorie Sonnay, Felix Zelder
This communication describes the stabilizing effect (ΔΔG° = -4 kJ mol-1) of a remote methyl group in the backbone of a cobalamin-enzyme mimic on intramolecular imidazole-cobalt coordination. For this purpose, two B12 derivatives with an appended imidazole base were synthesized and analysed with spectrophotometric pH titrations. Qualitative conformation analysis of the backbone structure suggests that a thermodynamically unfavoured gauche interaction in the base-off form of a model containing an (R)-configured CH3 group at position C176 of the linker between the corrin ring and the terminal imidazole ligand steers the base toward cobalt coordination...
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30019723/structures-electronic-properties-reactivity-and-dynamic-studies-of-three-new-polyoxometalate-compounds
#9
Ali Harchani, Monika Kučeráková, Michal Dušek, Amor Haddad
We report a complex study on the crystal structures, electronic properties, reactivity and dynamics of three polyoxometalate compounds (C6NH8)4[H2P2Mo5O23]·5H2O (1), (C2H8N)5[HP2Mo5O23]·(C3H9NO2)0.5·(H2O)1.5 (2) and (C2H8N)3[PMo12O40]·(H2O)0.34 (3). These compounds were synthesized using a solution method and characterized by single-crystal X-ray diffraction. Crystallography confirmed three distinct symmetries P1[combining macron], P21/c and R3[combining macron]c for 1, 2, and 3, respectively, and unit cell constants a = 12...
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30019721/ionic-columnar-clustomesogens-associations-between-anionic-hexanuclear-rhenium-clusters-and-liquid-crystalline-triphenylene-tethered-imidazoliums
#10
F Camerel, F Kinloch, O Jeannin, M Robin, S K Nayak, E Jacques, K A Brylev, N G Naumov, Y Molard
Providing several functionalities to a single material is an emerging challenge with many industrial prospects in materials sciences. Self-assembled organic-inorganic hybrid materials endowed with emission properties are part of these new materials. While the inorganic moieties provide emissivity, the organic part confers nanostructuration and processability. Here we describe how columnar arrangements can be obtained by assembling, via electrostatic interactions, isometric anionic inorganic nanoemitters, namely [Re6Se8(CN)6]4-, with imidazolium counter cations bearing triphenylene units...
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30019062/ferritin-encapsulation-of-artificial-metalloenzymes-engineering-a-tertiary-coordination-sphere-for-an-artificial-transfer-hydrogenase
#11
Martina Hestericová, Tillmann Heinisch, Markus Lenz, Thomas R Ward
Ferritin, a naturally occuring iron-storage protein, plays an important role in nanoengineering and biomedical applications. Upon iron removal, apoferritin was shown to allow the encapsulation of an artificial transfer hydrogenase (ATHase) based on the streptavidin-biotin technology. The third coordination sphere, provided by ferritin, significantly influences the catalytic activity of an ATHase for the reduction of cyclic imines.
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30019052/oxide-sulfide-based-hybrid-arrays-as-robust-electrocatalysts-for-water-splitting
#12
Xiaoqiang Du, Qibin Wang, Yu Li, Xiaoshuang Zhang
It is imperative to develop bifunctional electrocatalysts with good activity and stability for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). In this paper, a hierarchical NiCo2O4/Ni3S2 hybrid is synthesized by direct growth on nickel foam (NF) using co-precipitation and sulfuration as a general two-step method. When the NiCo2O4/Ni3S2/NF material is used as an electrode, it displays high activity and perfect stability for OER. A low overpotential of only 360 mV is obtained at 40 mA cm-2, comparable to the benchmark of IrO2 electrodes (330 mV overpotential at 40 mA cm-2), benefiting from the particular hybrid structure of NiCo2O4/Ni3S2/NF with large surface area and fast electron transfer...
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30019047/normal-and-abnormal-nhc-coordination-in-cationic-hydride-iodide-complexes-of-aluminium
#13
Michael Trose, Stuart Burnett, Simon J Bonyhady, Cameron Jones, David B Cordes, Alexandra M Z Slawin, Andreas Stasch
The mixed N-heterocyclic carbene (NHC) complexes NHCAlHxI3-x, where NHC is IDip or IMes ((HCNAr)2C:, Ar = 2,6-iPr2C6H3 = Dip (IDip); or 2,4,6-Me3C6H2 = Mes (IMes)), x = 1 or 2, were either prepared from NHCAlH3 and NHCAlI3 or by halogenation of NHCAlH3 with MeI. Reaction of [(IDip)AlHxI3-x], with x = 0-3, with another equivalent of IDip afforded either fluxional equilibria in benzene solution for x = 0, no reaction for x = 3, or the new mixed normal-abnormal NHC-coordinated ionic complexes [(IDip)AlH2(aIDip)]I (9) and [(IDip)AlHI(aIDip)]I (10), where aIDip is the abnormal IDip carbene tautomer bonded through its 4-position...
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30019045/a-3d-moo-x-carbon-composite-array-as-a-binder-free-anode-in-lithium-ion-batteries
#14
Tim Herdt, Michael Bruns, Jörg J Schneider
Molybdenum(vi) oxide (MoO3) nanorod arrays were synthesized employing a template-assisted method. A polycarbonate membrane as a template was vacuum infiltrated with an aqueous solution of ammonium heptamolybdate. Template removal by oxygen plasma etching and calcination leads to the formation of highly crystalline 3D MoO3 nanorod arrays as a negative replica of the template. By applying sucrose as the carbon precursor, the mantling of the MoO3 nanorods with a thin carbon coating is obtained. Simultaneously, the direct and binder-free contact between the 3D MoOx nanorod arrays and the current collector resulting from the carbon coating could be achieved and leads to high capacities of up to 1376, 783, 856, 804 and 324 mA h g-1 for cycles 1, 2, 20, 50 and 200 as well as a coulombic efficiency of 99% for such 3D MoOx/C composite electrodes...
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30019042/nitrogen-doped-graphene-like-carbon-nanosheets-from-commercial-glue-morphology-phase-evolution-and-li-ion-battery-performance
#15
D Damodar, S Krishna Kumar, S K Martha, A S Deshpande
We report a two-step process to synthesize nitrogen-doped graphene-like carbon nanosheets (N-CNS), using commercially available ethyl cyanoacrylate based super glue as a carbon precursor. In this process, super glue is polymerized in aqueous NaCl solution, followed by carbonization at 1000 °C. Scanning electron microscopy (SEM) and high resolution transmission electron microscopy (HRTEM) studies show that the resultant material consists of micron-sized carbon nanosheets with a wrinkled morphology. HRTEM, X-ray diffraction (XRD), XPS and Raman spectroscopic studies confirm the formation of nanocrystalline and graphitic, nitrogen-doped carbon nanosheets...
July 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30015821/synthesis-and-thermoelastic-properties-of-zr-cn-2-2-and-hf-cn-2-2
#16
Konstantin Dolabdjian, Arne Kobald, Carl P Romao, Hans-Jürgen Meyer
Two binary transition metal cyanamides, Zr(CN2)2 and Hf(CN2)2, were prepared by solid-state metathesis (SSM) reactions and separately controlled by differential thermoanalysis (DTA). The crystal structure of Hf(CN2)2 was solved and refined from a single-phase crystal powder by X-ray diffraction (XRD) in the space group Pbcn. Zr(CN2)2 was characterized by isotypic indexing. The crystal structure of M(CN2)2 compounds with M = Zr, Hf is closely related to that of LiY(CN2)2, but reveals large cavities due to the absence of lithium ions...
July 17, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30015820/stimuli-responsive-metal-organic-supercontainers-as-synthetic-proton-receptors
#17
Cheng-Zhe Sun, Li-Ji Cheng, Yupu Qiao, Li-Yi Zhang, Zhong-Ning Chen, Feng-Rong Dai, Wei Lin, Zhenqiang Wang
We demonstrate a proof-of-concept design of a new platform for proton recognition and modulation. The new proton receptors are derived from a unique class of synthetic supercontainers that exhibit exceptional proton binding capacity (over 50 equiv.) and intriguing proton-dependent fluorescent switching behavior. Experimental and computational studies suggest that the proton-responsive event involves a two-step mechanism pertaining to proton binding by both amino and pyrenyl moieties of the supercontainer constructs...
July 17, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30015819/a-new-diphosphine-carbonyl-complex-of-ruthenium-an-efficient-precursor-for-c-c-and-c-n-bond-coupling-catalysis
#18
Aparajita Mukherjee, David A Hrovat, Michael G Richmond, Samaresh Bhattacharya
Reaction of 1,2-bis(diphenylphosphino)benzene (dppbz) with [{Ru(CO)2Cl2}n] affords [Ru(dppbz)(CO)2Cl2], where the two carbonyls are mutually cis and the two chlorides are trans. The molecular structure of [Ru(dppbz)(CO)2Cl2], has been determined by X-ray crystallography, and the stability of the different available stereoisomers has been computationally evaluated. [Ru(dppbz)(CO)2Cl2] has been found to serve as an excellent pre-catalyst for catalytic Suzuki-type C-C coupling and Buchwald-type C-N coupling reactions...
July 17, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30015817/nuclearity-effects-in-supported-single-site-fe-ii-hydrogenation-pre-catalysts
#19
Ryan R Langeslay, Hyuntae Sohn, Bo Hu, Jacob S Mohar, Magali Ferrandon, Cong Liu, Hacksung Kim, A Jeremy Kropf, Ce Yang, Jens Niklas, Oleg G Poluektov, E Ercan Alp, Patricia Ignacio-de Leon, Alfred P Sattelberger, Adam S Hock, Massimiliano Delferro
Dimeric and monomeric supported single-site Fe(ii) pre-catalysts on SiO2 have been prepared via organometallic grafting and characterized with advanced spectroscopic techniques. Manipulation of the surface hydroxyl concentration on the support influences monomer/dimer formation. While both pre-catalysts are highly active in liquid-phase hydrogenation, the dimeric pre-catalyst is ∼3× faster than the monomer. Preliminary XAS experiments on the H2-activated samples suggest the active species are isolated Fe(ii) sites...
July 17, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/30014082/facile-incorporation-of-technetium-into-magnetite-magnesioferrite-and-hematite-by-formation-of-ferrous-nitrate-in-situ-precursors-to-iron-oxide-nuclear-waste-forms
#20
Wayne W Lukens, Sarah A Saslow
The fission product, 99Tc, presents significant challenges to the long-term disposal of nuclear waste due to its long half-life, high fission yield, and to the environmental mobility of pertechnetate (TcO4-), the stable Tc species in aerobic environments. Migration of 99Tc from disposal sites can potentially be prevented by incorporating it into durable waste forms based on environmentally stable minerals. Since Tc(iv) and Fe(iii) have the same ionic radius, Tc(iv) can replace Fe(iii) in iron oxides. Environmentally durable iron oxides include goethite (α-FeOOH), hematite (α-Fe2O3), and magnesioferrite (MgFe2O4)...
July 17, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
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