研究领域

Inorganic Chemistry

Research in the Weller group is based upon synthetic organometallic chemistry, and in particular the generation and stabilisation of transition metal complexes with a low coordination number. Through this we are interested in topics related to catalysis, structure and bonding and energy, and in particular complexes that display C-H, B-H and C-C bonding modes (via agostic and sigma interactions) and activation. We also have interest in the self-assembly of metal fragments to form novel clusters that show promise as models for hydrogen on metal surfaces, hydrogen storage devices and models for nanoparticles. Please follow the link to our Research Group Webpages for more information on the group, its research and our publications. Current Research Themes: (1) The synthesis and definitive characterisation of late transition metal C-C and B-H and C-H sigma and agostic complexes. These complexes also undergo C-C, B-H and C-H activation in solution, making them genuine intermediates in these transformations of growing synthetic utility. Highlights include the isolation of complexes with C-C agostic interactions, [1, 2] alkyl dehydrogenation and C-H activation, [3,4] and the unraveling of the mechanism of dehydrocoupling of amine boranes: precursors to chemical hydrogen stores for fuel cell applications and novel B-N polymeric materials.[5,6,7] (2) The role of hemilabile ligands in stabilising latent vacant coordination sites on transition metal systems. A recent important result from this work is the development (with Willis, Oxford) of hydroacylation catalysts for challenging substrates (C-H activation) in which each steps on the catalytic cycle has been characterized.[8, 9] (3) The synthesis of a new class of unsaturated metal clusters [10,11,12], by a kinetically-controlled self-assembly process, which have an extraordinarily high hydride content; are models for hydrogen attachment on a metal surface; uptake and release H2; undergo a variety of electrochemical processes due their unsaturated electronic structure and act as redox-switchable hydrogen storage materials.

近期论文

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G. M. Adams, F. M. Chadwick, S. D. Pike and Andrew S. Weller* A CH2Cl2 Complex of a [Rh(pincer)]+ Cation, Dalton Trans., 2015, in the press (special issue dedicated to Professor Ken Wade). S. D. Pike, T. Krämer N. H. Rees, S. A. Macgregor,* A. S. Weller* Stoichiometric and Catalytic Solid–Gas Reactivity of Rhodium Bis–Phosphine Complexes. Organometallics 2015, in the press. P. Ren, S. D. Pike, I. Pernik, A. S. Weller* and M.C. Willis Rh–POP Pincer Xantphos Complexes for C–S and C–H Activation. Implications for Carbothiolation Catalysis. Organometallics 2015, in the press. S. D. Pike, F. M. Chadwick, N. H. Rees, M. P. Scott, A. S. Weller,* T. Krämer, and S. A. Macgregor* Solid–State Synthesis and Characterization of Sigma−Alkane Complexes, [Rh(L2)(η2,η2–C7H12)][BArF4] (L2 = Bidentate Chelating Phosphine). J. Am. Chem. Soc. 2015, 137, 820 H. C. Johnson, T. N. Hooper and A. S. Weller The Catalytic Dehydrocoupling of Amine– and Phopshine– Boranes, Top. Organomet. Chem. 2015, 49, 153. S. D. Pike,* I. Pernik, R. Theron, J. S. McIndoe,* A. S. Weller* Relative Binding Affinities of Fluorobenzene Ligands in Cationic Rhodium Bisphosphine η6 Fluorobenzene Complexes Probed Using Collision-Induced Dissociation. J. Organometallic Chem. 2015 in the press. S. D. Pike* and A. S. Weller* Organometallic Synthesis, Reactivity and Catalysis in the Solid–State Using Well–Defined Single Site Species, Phil. Trans. R. Soc. A, 2015 373 20140187 (Invited contribution). H. C. Johnson, R. Torry-Harris, L. Ortega, R. Theron, J. S. McIndoe and Andrew S. Weller* Exploring the Mechanism of the Hydroboration of Alkenes by Amine-Boranes Catalysed by [Rh(Xantphos)]+ Catal. Sci. Technol. 2014, 4, 3486 H. C. Johnson, E. M. Leitao, G. R. Whittell, I. Manners,* G. C. Lloyd-Jones,* and A.S. Weller* Mechanistic Studies of the Dehydrocoupling and Dehydropolymerization of Amine-Boranes using a [Rh(Xantphos)]+ Catalyst J. Am. Chem. Soc. 2014, 136, 9078. A. Kumar, H. C. Johnson, T. N. Hooper, A. S. Weller,* A.G. Algarra and S. A. Macgregor* Multiple metal-bound oligomers from Ir-catalysed dehydropolymerisation of H3BNH3 as probed by experiment and computation Chem. Sci. 2014, 5, 2546. T. N. Hooper, M. A. Huertos, T. Jurca, S. D. Pike, A. S. Weller,* I. Manners The Effect of the Phosphine Steric and Electronic Profile on the Rh–Promoted Dehydrocoupling of Phosphine-Boranes, Inorg. Chem. 2014, 53, 3716 A.G. Algarra, L. J. Sewell, H. C. Johnson, S. A. Macgregor,* A.S. Weller* A Combined Experimental and Computational Study of Fluxional Process in Sigma Amine–Borane Complexes of Rhodium and Iridium, Dalton Trans. 2014, 43, 11118. M. Etienne* and A. S. Weller* Intramolecular C–C agostic complexes: C–C sigma interactions by another name Chem. Soc. Rev. 2014, 43, 242. S. D. Pike and A. S. Weller* C–Cl Activation of the Weakly Coordinating Anion B(3,5–Cl2C6H3)4]– at a Rh(I) Centre in Solution and the Solid–State Dalton Trans. 2013, 42, 12832. H. C. Johnson, C. L. McMullin, S. D. Pike, S.A. Macgregor* and A. S. Weller* Dehydrogenative B–B Homocoupling of an Amine–Borane Angew. Chem. Int. Ed. 2013, 42, 9776. T. A. Shuttleworth, M. A. Huertos, I.Pernik, R. D. Young, A. S. Weller* Bis(phosphine)boronium salts. Synthesis, Structures and Co-ordination Chemistry Dalton Trans. 2013, 42, 12917. L. J. Sewell, M. A. Huertos, M. E. Dickinson and A. S. Weller,* G. C. Lloyd–Jones Dehydrocoupling of Dimethylamine Borane Catalysed by Rh(PCy3)2H2Cl Inorg. Chem. 2013, 52, 4509. M. A. Huertos and A. S. Weller* Revealing the P–B coupling event in the rhodium catalysed dehydrocoupling of phosphine boranes H3B·PR2H (R = tBu, Ph). Chem. Sci. 2013, 4, 1881. J. F. Hooper, R. D. Young, I. Pernik, A. S. Weller* and M. C. Willis* Carbon-carbon bond construction using boronic acids and aryl methyl sulfides: Orthogonal reactivity in Suzuki-type couplings Chem. Sci. 2013, 4, 1568. J. F. Hooper, R. D. Young, A. S. Weller and M. C. Willis* Traceless chelation-controlled rhodium-catalysed intermolecular alkene and alkyne hydroacylation, Chem. Eur. J. 2013 19, 3125.