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Unsymmetrical Iron P-NH-P' Catalysts for the Asymmetric Pressure Hydrogenation of Aryl Ketones.
2017
R.H.M. thanks NSERC Canada for a Discovery grant and the Canada Council for the Arts for a Killam Fellowship. This work was also made possible by the SCICOMP NMR facilities provided by the Canada Foundation for Innovation, project number 19119, and the Ontario Ministry of Research, Innovation and Science. The Deutscher Akademischer Austauschdienst (DAAD) is thanked for support for A.P. Calculations were performed using the facilities of SHARCNET and Scinet of Compute/Calcul Canada
A decacobalt(ii) cluster with triple-sandwich structure obtained by partial reductive hydrolysis of a pentacobalt(ii/iii) Weakley-type polyoxometalat…
2016
Partial reductive hydrolysis of a penta-CoII/III cluster [CoII4(H2O)2(CoIIIW9O34)(PW9O34)]12− (1) leads to the formation of [Co2{Co3(H2O)(Co(OH)2W7O26)(PW9O34)}2]22− (2). This polyoxometalate is made up of two capping [PW9O34]9− units and two bridging [W7O26]10− units that assemble to encapsulate a novel deca-CoII cluster core comprising octahedral and tetrahedral CoII ions.
Light-Induced Alkylation of (Hetero)aromatic Nitriles in a Transition-Metal-Free C–C-Bond Metathesis
2017
A light-induced C–C-σ-bond metathesis was achieved through transition-metal-free activation of an unstrained C(sp3)–C(sp3)-σ-bond in 1-benzyl-1,2,3,4-tetrahydroisoquinolines. A photoredox-mediated single-electron oxidation of these precursor amines yield radical cations which undergo a homolytic cleavage of a C(sp3)–C(sp3)-σ-bond rather than the well-known α-C–H-scission. The resulting carbon-centered radicals are used in the ipso-substitution of (hetero)aromatic nitriles proceeding through another single-electron transfer-mediated C–C-bond cleavage and formation.
Amino‐Substituted Ferra‐bis(tricarbollides) − Metallatricarbaboranes Designed for Linear Molecular Constructions
2004
Reactions between high purity FeCl2 and the anion [nido-7-(tBuHN)-7,8,9-C3B8H10)]− (1−) have been used for efficient syntheses of the twelve-vertex double-cluster metallatricarbollide complexes of the para,para (p,p) type [closo-9,9′(RHN)2-commo-2,2′-FeII-1,7,9-(C3B8H10)-1′,7′,9′-(C3B8H10)] (2) (2a, R = tBu and 2b, R = H) (yields 42−45% for 2a). Compound 2b, which contains two reactive amino substituents conveniently attached to the tricarbollide subclusters in p-positions with respect to the metal center, was prepared via facile cleavage of the tBu substituent in 2a either by AlCl3 or by thermal means. The structure of 2b constitutes a good setting for the synthesis of building blocks for …
Magnetostructural correlations in CuII−NC−WV linkage: the case of [CuII(diimine)]2+−[WV(CN)8]3− 0D assemblies
2009
International audience; We report on the syntheses, crystal structures, and magnetic properties of two cyano-bridged molecular assemblies: [CuII(phen)3]2{[CuII(phen)2]2[WV(CN)8]2}(ClO4)2·10H2O (phen = 1,10-phenanthroline) (1) and {[CuII(bpy)2]2[WV(CN)8]} {[CuII(bpy)2][WV(CN)8]}·4H2O (bpy = 2,2′-bipyridyl) (2). Compound 1 consists of cyano-bridged [CuII2WV2]2− molecular rectangles and isolated [CuII(phen)3]2+ complexes. The molecular structure of 2 reveals cyano-bridged trinuclear [CuII2WV]+ and dinuclear [CuIIWV]− ions. Magnetic interactions in 1 are interpreted in terms of the model of a tetranuclear moiety consisting of two ferromagnetic CuII−NC−WV units (J1 = +39(4) cm−1) interacting ant…
Cobalt Clusters with Cubane-Type Topologies Based on Trivacant Polyoxometalate Ligands.
2016
Four novel cobalt-substituted polyoxometalates having cobalt cores exhibiting cubane or dicubane topologies have been synthesized and characterized by IR, elemental analysis, electrochemistry, UV-vis spectroscopy, X-ray single-crystal analysis, and magnetic studies. The tetracobalt(II)-substituted polyoxometalate [Co4(OH)3(H2O)6(PW9O34)](4-) (1) consists of a trilacunary [B-α-PW9O34](9-) unit which accommodates a cubane-like {Co(II)4O4} core. In the heptacobalt(II,III)-containing polyoxometalates [Co7(OH)6(H2O)6(PW9O34)2](9-) (2), [Co7(OH)6(H2O)4(PW9O34)2]n(9n-) (3), and [Co7(OH)6(H2O)6(P2W15O56)2](15-) (4), dicubane-like {Co(II)6Co(III)O8} cores are encapsulated between two heptadentate [B…
Computational Study of the Effect of Glyoxal–Sulfate Clustering on the Henry’s Law Coefficient of Glyoxal
2014
We have used quantum chemical methods to investigate the molecular mechanism behind the recently reported ( Kampf , C. J. ; Environ. Sci. Technol . 2013 , 47 , 4236 - 4244 ) strong dependence of the Henry's law coefficient of glyoxal (C2O2H2) on the sulfate concentration of the aqueous phase. Although the glyoxal molecule interacts only weakly with sulfate, its hydrated forms (C2O3H4 and C2O4H6) form strong complexes with sulfate, displacing water molecules from the solvation shell and increasing the uptake of glyoxal into sulfate-containing aqueous solutions, including sulfate-containing aerosol particles. This promotes the participation of glyoxal in reactions leading to secondary organic…
The roles of microlites and phenocrysts during degassing of silicic magma
2022
Abstract Silicic magmas span a wide range of eruptive styles between explosive and effusive, and transitions between these styles are commonplace. Yet the triggers of switches in eruptive style remain poorly understood. Eruptions are mostly driven by degassing of magmatic water and their eruption style - effusive or explosive - is likely governed by the efficiency of outgassing as well as magma ascent rate. Microlites and phenocrysts are often purported to promote heterogeneous bubble nucleation and outgassing, both key variables in the degassing dynamics that become crucial in controlling the eruptive style. Here, in order to shed light on the role of nature, size and abundance of crystals…
Environmental change during the Early Cretaceous in the Purbeck-type Durlston Bay section (Dorset, Southern England): a biomarker approach.
2007
20 pages; International audience; The Purbeck-type section (Durlston Bay, Dorset, UK) exhibits littoral lagoonal to lacustrine facies. It shows a gradual climatic/environmental change from semi-arid conditions associated with evaporites at the Jurassic–Cretaceous transition, to a more humid climate at the end of the Berriasian. Though generally organic-poor (total organic carbon, TOC, <1.3%), the Durlston Bay section shows an organic-rich episode (TOC up to 8.5%) located at the transition from evaporitic to more humid facies. A biomarker study was performed in order to determine the origin of the organic matter (OM) in the section and see if changes in organic sources accompanied the genera…
Pre- and syn-eruptive geochemistry of volcanic gases from Soufriere Hills of Montserrat, West Indies
1998
International audience; Soufriere Hills fumaroles contained magmaderived volatiles before and during the eruption initiated in 1995 but also preserved a typical and quite steady hydrothermal coinposition. Chemical changes due to increased boiling and a greater input of oxidizing magmatic gas occurred only at Galway's Soufriere, the most active fumarolic field. Hydrothermal buffering of the fumaroles has been favoured by their remote location (!-2 km) froin the eruptive vents and by a preferential degassing of the uprising magma through intrusive conduits under the crater. High temperature (720øC) gas collected froin the extruding lava dome in Feb. 1996 was chemically and isotopically repres…