Monomeric Iron and Cobalt Compounds with Cyanide and Isocyanide Ligands PDF Download
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Author: Anthony John Pesiri
Publisher:
ISBN:
Category : Hydrogenase
Languages : en
Pages :
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Author: Anthony John Pesiri
Publisher:
ISBN:
Category : Hydrogenase
Languages : en
Pages :
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Author: Charles Cameron Mokhtarzadeh
Publisher:
ISBN:
Category :
Languages : en
Pages : 434
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This dissertation describes the targeted attempts at the generation of transition metal species that function as precise electronic structure mimics to the well known spin triplet (S =1) metal carbonyls fragments Fe(CO)4 and CpCo(CO). These unsaturated fragments have been shown to display a wide range reactivity, and competency towards important reaction chemistry such as alkane and N2 binding, and E-H bond activation due to a unique interplay of a strong ligand field, formal dn count, and orbital symmetry, rendering these fragments primed for bond activation. Accordingly, ligand architectures that can accurately mimic the ligand field provided by CO to kinetically stabilize these fragments could provide new inroads to novel small molecule activation pathways. To this end, sterically encumbering m-terphenyl isocyanides serve as isolobal ligand surrogates for carbon monoxide (CO). Additionally isocyanides have the added benefit of providing kinetic stabilization by virtue of readily tunable isocyano-R (CN-R) group. The first section of this dissertation describes the synthesis and protonation of an encumbered tetra-isocyanide iron dianion, Na2[Fe(CNArMes2)4] (ArMes2 = 2,6-(2,4,6 --Me3C6H2)2C6H3), which serves as a platform for targeting species of the formulation Fe(CNArMes2)4. It is shown that the reactivity of the electronically unsaturated Fe(CNR)4 fragment upon protonation of Na2[Fe(CNArMes2)4] and subsequent alkylation of Na[HFe(CNArMes2)4], yields the dinitrogen stabilized species Fe(N2)(CNArMes2)4. Fe(N2)(CNArMes2)4 is shown to readily undergo intramolecular C-H activation of the ligand scaffold upon liberation N2 under ambient conditions purportedly through and insipient [Fe(CNArMes2)4] fragment. Further more, ability of Na2[Fe(CNArMes2)4] to facilitate the reductive disproportionation of CO2, in addition to CO2 capture with electrophilic silyl sources is presented culminating in a rare class of low valent Fe-aminocarbyne complexes. The second vignette of this dissertation focuses on the generation of species that mimic the formulation CpCo(L). It is shown that with less encumbering m-terphenyl isocyanides that aggregation akin to the unsaturated carbonyl congeners is realized. Use of encumbering m-terphenyl isocyanides provides access to the three memebered electron transfer series [([mu]2-CNArMes2)2[CpCo]2]n (n = 0,-1, -2). Notably, this series is the first of its kind to span all three ostensible electronic states (e.g. d8-d8, d8-d9, and d9-d9), previously unavailable with other [pi]-acidic ligand frameworks. Additionally this allows for a systematic reassessment of the metal-metal bonding within this class of dimeric species. Evidence is put forth in favor of no M-M bonding interactions occur within these systems and the integrity of the dimeric framework is in fact mitigated through a unique interplay of the metal d-manifold and the isocyanide [pi]*-system. Modulation of the steric profile of the m-terphenyl isocyanide and the Cp unit to Cp* so as to increase the steric pressure provides access to the first reported mono-nuclear Cp*Co(N2)L fragments. It is shown that these species function as viable sources of Cp*Co(CNR) for a number of bond activation processes including Si-H, H-H, and P-P bond scission. Moreover, the reactivity of these species culminates with the isolation of the second example of a structurally authenticated transition metal nitrous oxide (N2O) adduct, which exhibits an unprecedented [eta]2-(N,N) coordination mode to Co. Finally, the reduction of the encumbered Cp*Co(CNArTripp2) (CNArTripp2 2,6-(2,4,6-(i-Pr)3C6H3)2C6H3) fragment provide access to the unique dianion K2[Cp*Co≡CNArTripp2]. It is shown that the dianion K2[Cp*Co≡CNArTripp2] exhibits 3-fold bonding between Co and the isocyanide -Ciso through an extreme case of M-->(CN) [pi]*-back donation and gives rise to the first example of a Co-carbyne complex. The reactivity and electronic structure are presented for K2[Cp*Co≡CNArTripp2] and it is concluded that this reactive dianion behaves as a potent metal based nucleophile and source of [Cp*Co(CNR)]2- for a number of bond activation process.
Author: D. Nicholls
Publisher: Elsevier
ISBN: 148314643X
Category : Science
Languages : en
Pages : 201
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The Chemistry of Iron, Cobalt and Nickel deals with the chemistry of iron, cobalt, and nickel and covers topics ranging from the occurrence and distribution of all three elements to their properties, allotropy, and analytical chemistry. Compounds of iron, cobalt, and nickel in both low and high oxidation states are also discussed. This book is divided into three sections and begins with the history of iron, along with its occurrence and distribution, allotropy, and preparation and industrial production. The nuclear, physical, and chemical properties of iron, as well as the biological importance of iron compounds, are also considered. Compounds of iron are discussed, including carbonyls and nitric oxide complexes. The next two sections deal with the history, occurrence and distribution, allotropy, analytical chemistry, and preparation and industrial production of cobalt and nickel, along with their nuclear, physical, and chemical properties. Compounds of cobalt and nickel are examined, from carbonyls and nitrosyls to cyanides and organometallic compounds. This monograph will be a useful resource for inorganic chemists.
Author: Julian A. Davies
Publisher: World Scientific
ISBN: 9789810220846
Category : Science
Languages : en
Pages : 482
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Although coordination chemistry naturally centers on the synthesis of coordination compounds, the synthesis of these materials is typically not an end in itself. Coordination compounds are utilized in all branches of chemistry; from theoretical modeling to industrial and consumer products. While a large amount of information is available on coordination chemistry in general and synthetic methods in particular, no comprehensive work has been presented on the preparation of coordination compounds with an emphasis on synthetic strategies rather than on detailed descriptions of specific syntheses. The goal of this book is to provide an approach to coordination chemistry that is based upon preparative strategies.The main aim of the authors is to present a systematic classification of synthetic reactions rather than an encyclopedic listing of experimental results. Hence, the coverage is more selective than exhaustive. Despite this, the book provides access to the original literature with ca. 2000 references. The edition is well-illustrated and contains almost 250 schemes, figures and illustrations of crystal structures of selected complexes.
Author: Chemical Society (Great Britain)
Publisher:
ISBN:
Category : Chemistry
Languages : en
Pages : 1214
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Author: American Chemical Society. Meeting
Publisher:
ISBN:
Category : Chemistry
Languages : en
Pages : 1398
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Author:
Publisher:
ISBN:
Category : Dissertations, Academic
Languages : en
Pages : 664
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Author: Marco Montalti
Publisher: CRC Press
ISBN: 1420015192
Category : Science
Languages : en
Pages : 662
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Since the publication of the second edition of this handbook in 1993, the field of photochemical sciences has continued to expand across several disciplines including organic, inorganic, physical, analytical, and biological chemistries, and, most recently, nanosciences. Emphasizing the important role light-induced processes play in all of these fie
Author: A. G. Sharpe
Publisher:
ISBN:
Category : Medical
Languages : en
Pages : 328
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Author:
Publisher:
ISBN:
Category : Medicine
Languages : en
Pages : 1318
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