The Synthesis, Characterization, and Reactivity of First-row Late Transition Metal Complexes Containing Tridentate Pincer-type N-heterocyclic Phosphenium Ligands PDF Download
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Author: Sadie E. Knight
Publisher:
ISBN:
Category : Ligand binding (Biochemistry)
Languages : en
Pages : 276
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Author: Sadie E. Knight
Publisher:
ISBN:
Category : Ligand binding (Biochemistry)
Languages : en
Pages : 276
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Author: Baofei Pan
Publisher:
ISBN:
Category : Ligands
Languages : en
Pages : 175
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Author: Bailey Jeanne Jackson
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Category :
Languages : en
Pages :
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Author: Adam Ruddy
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Category :
Languages : en
Pages :
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Author: John C. Linehan
Publisher:
ISBN:
Category :
Languages : en
Pages : 514
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![Synthesis and Reactivity of Transition Metal Complexes Bearing the Tridentate Bis(2-mercapto-p-tolyl)amine ([SNS]H 3) Ligand PDF](https://books.google.com/books/content/images/frontcover/yhZvswEACAAJ?fife=w80-h100)
Author: Kyle Evan Rosenkoetter
Publisher:
ISBN: 9780355307856
Category :
Languages : en
Pages : 196
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The work described herein focuses on the synthesis and characterization of new heterobimetallic complexes containing the redox-active W[SNS] 2 metalloligand and investigation into their electronic properties and reactivity. Most recent studies have explored the redox nature of the [SNS]H 3 scaffold through the synthesis and reactivity of a novel set of square-planar nickel complexes.Chapters 2 and 3 describe a modular synthetic approach towards generating a new series of heterobimetallic complexes with the general formula W[SNS]2M(L) ([SNS] = bis(2-mercapto- p-tolyl)amine; M = Ni, Pd, or Pt; and L = dppe, depe, dmpe, dppp, PR'2NRPR'2 (R = phenyl, benzyl; R'=phenyl), DPEphos or dppf). The complexes were prepared by a salt metathesis of Cl2MII(L) with the previously reported W[SNS]2 coordination complex under reducing conditions. X-ray diffraction analysis revealed interesting coordination geometries about the appended Group 10 metal centers moving from Pt and Pd (pseudo-square planar) to the first row Ni (pseudo-tetrahedral) analogue. These complexes demonstrate formal metal--metal bond formation across the series with a tunable first oxidation potential up to 600 mV.Chapter 4 investigates the use of W[SNS]2Ni(dppe) as a catalyst for the electrochemical reduction of protons to hydrogen. This complex was found to catalytically generate hydrogen with an overpotential of 700 mV, a TOF of 14 sec--1, and a Faradaic yield of 80 +/- 3 % using 4-cyanoanilinium tetrafluoroborate in non-aqueous solutions.Chapter 5 demonstrates the effect of exchanging the nickel center of the heterobimetallic complexes discussed in Chapters 2 and 3 with other first row transitions metal ions (i.e. cobalt and copper). Analysis into the observed metal--metal distances reveal stark differences across the series. Additionally, the copper ion containing complexes demonstrate dynamic behavior in solution.Chapter 6 investigates the synthesis and reactivity of a series of monomeric square-planar nickel complexes of the [SNS] scaffold to demonstrate the ligand as redox, proton, and hydrogen atom non-innocent.Appendix A illustrates the electrochemical responses observed for the monoanionic complexes from Chapter 6 in the presence of CO2 and CO. Appendices B and C describe the synthesis and characterization of a five-coordinate cobalt and a heterotrimetallic tungsten-nickel complex, respectively.
Author: Brenda Frazier
Publisher:
ISBN:
Category :
Languages : en
Pages : 0
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Author: Nathaniel C. McCutcheon
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ISBN:
Category : Chemistry, Inorganic
Languages : en
Pages : 0
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In light of growing environmental and economic concerns, there is a motivated effort to mimic the two-electron reactivity of precious transition metal complexes using more abundant, affordable, and non-toxic first row transition metals. The main challenge in this effort is that more sustainable first row transition metals do not readily undergo two-electron redox processes, which comprise many industrially relevant catalytic mechanisms, instead preferring to participate in one-electron reactions. One of several ways the Thomas group has approached this challenge is by tethering a Lewis acidic early metal to an electron-rich late metal via a bifunctional phosphinoamide ligand framework, allowing access to highly reduced late metal centers that have been shown to more favorably undergo two-electron redox processes. This thesis explores how the electron-donating properties of the phosphinoamide ligand impact the structure and reactivity of a novel series of bis(phosphinoamide) Zr/Co complexes. This series employs a more electron-donating iPrNPiPr2- ligand, as opposed to the XylNPiPr2- ligand previously featured in the group’s bis(phosphinoamide) Zr/Co systems. The relative electron density at the cobalt center is qualified using multiple spectroscopic and computational methods, and structural comparisons are made between analogous Zr/Co complexes bearing different ligands. These data are used to determine how increasing the electron-donating ability of the bis(phosphinoamide) framework impacts the thermodynamics of bond activation and the overall structure-reactivity relationship of Zr/Co complexes.
Author: Sarah Mcdougall
Publisher:
ISBN:
Category :
Languages : en
Pages : 0
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Author:
Publisher:
ISBN:
Category :
Languages : en
Pages : 122
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