Control of cerium oxidation state through metal complex secondary structures

Levin, Jessica R.; Dorfner, Walter L.; Carroll, Patrick J.; Schelter, Eric J.

doi:10.1039/C5SC02607E

Title: Control of cerium oxidation state through metal complex secondary structures

Abstract

A series of alkali metal cerium diphenylhydrazido complexes, M_x(py)_y[Ce(PhNNPh)₄], M = Li, Na, and K, x = 4 (Li and Na) or 5 (K), and y = 4 (Li), 8 (Na), or 7 (K), were synthesized to probe how a secondary coordination sphere would modulate electronic structures at a cerium cation. The resulting electronic structures of the heterobimetallic cerium diphenylhydrazido complexes were found to be strongly dependent on the identity of the alkali metal cations. When M = Li⁺or Na⁺, the cerium(III) starting material was oxidized with concomitant reduction of 1,2-diphenylhydrazine to aniline. Reduction of 1,2-diphenylhydrazine was not observed when M = K⁺, and the complex remained in the cerium(III) oxidation state. Oxidation of the cerium(III) diphenylhydrazido complex to the Ce(_IV) diphenylhydrazido one was achieved through a simple cation exchange reaction of the alkali metals. As a result, UV-Vis spectroscopy, FTIR spectroscopy, electrochemistry, magnetic susceptibility, and DFT studies were used to probe the oxidation state and the electronic changes that occurred at the metal centre.

Authors:

Levin, Jessica R. ^[1]; Dorfner, Walter L. ^[1]; Carroll, Patrick J. ^[1]; Schelter, Eric J. ^[1]

Univ. of Pennsylvania, Philadelphia, PA (United States)

Publication Date:: Tue Aug 11 00:00:00 EDT 2015

Research Org.:: Univ. of Pennsylvania, Philadelphia, PA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Contributing Org.:: National Science Foundation (NSF), Washington, DC (United States)

OSTI Identifier:: 1221895

Grant/Contract Number:: SC0006518

Resource Type:: Journal Article: Accepted Manuscript

Journal Name:: Chemical Science

Additional Journal Information:: Journal Name: Chemical Science; Journal ID: ISSN 2041-6520

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Levin, Jessica R., Dorfner, Walter L., Carroll, Patrick J., and Schelter, Eric J. Control of cerium oxidation state through metal complex secondary structures.  United States: N. p., 2015. 
        Web.  doi:10.1039/C5SC02607E.

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                    Levin, Jessica R., Dorfner, Walter L., Carroll, Patrick J., & Schelter, Eric J. Control of cerium oxidation state through metal complex secondary structures.  United States.  https://doi.org/10.1039/C5SC02607E

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                    Levin, Jessica R., Dorfner, Walter L., Carroll, Patrick J., and Schelter, Eric J. 2015.  
        "Control of cerium oxidation state through metal complex secondary structures".  United States.  https://doi.org/10.1039/C5SC02607E.  https://www.osti.gov/servlets/purl/1221895.

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@article{osti_1221895,

  title        = {Control of cerium oxidation state through metal complex secondary structures},

  author       = {Levin, Jessica R. and Dorfner, Walter L. and Carroll, Patrick J. and Schelter, Eric J.},

  abstractNote = {A series of alkali metal cerium diphenylhydrazido complexes, Mx(py)y[Ce(PhNNPh)4], M = Li, Na, and K, x = 4 (Li and Na) or 5 (K), and y = 4 (Li), 8 (Na), or 7 (K), were synthesized to probe how a secondary coordination sphere would modulate electronic structures at a cerium cation. The resulting electronic structures of the heterobimetallic cerium diphenylhydrazido complexes were found to be strongly dependent on the identity of the alkali metal cations. When M = Li+ or Na+, the cerium(III) starting material was oxidized with concomitant reduction of 1,2-diphenylhydrazine to aniline. Reduction of 1,2-diphenylhydrazine was not observed when M = K+, and the complex remained in the cerium(III) oxidation state. Oxidation of the cerium(III) diphenylhydrazido complex to the Ce(IV) diphenylhydrazido one was achieved through a simple cation exchange reaction of the alkali metals. As a result, UV-Vis spectroscopy, FTIR spectroscopy, electrochemistry, magnetic susceptibility, and DFT studies were used to probe the oxidation state and the electronic changes that occurred at the metal centre.},

  doi          = {10.1039/C5SC02607E},

  url          = {https://www.osti.gov/biblio/1221895},
  journal      = {Chemical Science},

  issn         = {2041-6520},

  number       = ,

  volume       = ,

  place        = {United States},

  year         = {Tue Aug 11 00:00:00 EDT 2015},

  month        = {Tue Aug 11 00:00:00 EDT 2015}

}

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Fig. 1: 30% probability thermal ellipsoid plots of Li₄(py)₄[Ce(PhNNPh)₄] (1) (left), Na₄(py)₈[Ce(PhNNPh)₄] (2) (middle), and K₅(py)₇[Ce(PhNNPh)₄] (3) (right) with the phenyl and pyridine rings shown in wire frame. Hydrogen atoms were omitted for clarity. Selected bond distances for 1 (Å): Ce(1)– N(1) 2.4408(13), Ce(1)–N(2) 2.4199(13), N(1)–N(2) 1.451(2), Li(2)–N(1) 2.018(3), Li(2)–N(10)more »

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Figures / Tables found in this record:

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Thermochemical cycles for water splitting employ thermal energy to drive a cyclic series of chemical reactions, the sum of which is just H/sub 2/O + thermal energy = H/sub 2/ + 1/2 O/sub 2/. It was shown previously that cerium (IV) oxide, CeO/sub 2/, reacts with alkali metal hydrogen phosphates - MH/sub 2/PO/sub 4/ or M/sub 2/HPO/sub 4/, where M = Li, Na, K - at > 600/sup 0/C to produce O/sub 2/(g), cerium(III) phosphate, CePO/sub 4/, and alkali metal orthophosphates, M/sub 3/PO/sub 4/. When M = Na or K, the double phosphate M/sub 3/Ce(PO/sub 4/)/sub 2/ forms from themore »« less
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Alkali metal cations often show pronounced ion specific interactions and selectivity with macromolecules in biological processes, colloids, and interfacial sciences, but a fundamental understanding about the underlying microscopic mechanism is still very limited. Here we report a direct probe of interactions between alkali metal cations (M{sup +}) and dicarboxylate dianions, O{sub 2}C(CH{sub 2})nCO{sub 2} (D{sub n}{sup 2-}) in the gas phase by combined photoelectron spectroscopy (PES) and ab initio electronic structure calculation on nine M{sup +}-D{sub n}{sup 2-} complexes (M = Li, Na, K; n = 2, 4, 6). PES spectra show that the electron binding energy (EBE) decreases frommore »« less
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Nuclear wastes generated from reprocessing of used nuclear fuel tend to contain a large fraction of rare earth (RE, e.g., Nd³⁺), transition (TM, e.g., Mo⁶⁺, Zr⁴⁺), alkali (A, e.g., Cs⁺), and alkaline earth cations (AE, e.g., Ba²⁺, Sr²⁺). Various strategies have been considered for immobilizing such waste streams, varying from nominally crystal-free glass to glass-ceramic to multi-phase ceramic waste forms. For glass and glass-ceramic waste forms, the added glass-forming system is generally alkali-alkaline earth-aluminoborosilicate (i.e., Na-Ca-Al-B-Si oxide). In a US-UK collaborative project, summarized here, we investigated the glass structure and crystallization dependence on compositional changes in simulated nuclear waste glassesmore »« less
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Title: Control of cerium oxidation state through metal complex secondary structures

Abstract

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Figures / Tables:

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Specific binding of cerium by human lactoferrin stimulates the oxidation of Ce3+ to Ce4+ journal, August 1994

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Reactivity of hydrazines with organometallic samarium complexes and the x-ray crystal structures of (C5Me5)2Sm(.eta.2-PhNHNPh)(THF), (C5Me5)2Sm(NHPh)(THF), and [(C5Me5)2Sm]2(.mu.-.eta.2:.eta.2-HNNH) journal, August 1992

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Diamagnetic Corrections and Pascal's Constants journal, April 2008

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Activity of CeOx and TiOx Nanoparticles Grown on Au(111) in the Water-Gas Shift Reaction journal, December 2007

Synthesis and Reactivity of a Ruthenium(III) Bis(anilide) Dimer by Oxidative Addition of an N,N‘-Disubstituted Hydrazine journal, July 2007

Molecular Structure and Magnetic Properties of Acetato-Bridged Lanthanide(III) Dimers journal, September 1995

Catalytic Cracking Reaction of Heavy Oil in the Presence of Cerium Oxide Nanoparticles in Supercritical Water journal, July 2013

Reduction of Hydrazines, Azo and Azoxy Compounds, and Amine N-Oxides with the NiCl2·2H2O–Li–DTBB (cat.) Combination journal, October 2000

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New perspective of electron transfer chemistry journal, January 2003

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New Scale Factors for Harmonic Vibrational Frequencies Using the B3LYP Density Functional Method with the Triple-ζ Basis Set 6-311+G(d,p)
journal, March 2005

Specific binding of cerium by human lactoferrin stimulates the oxidation of Ce3+ to Ce4+
journal, August 1994

Synthesis and Properties of High-Valent Organouranium Complexes Containing Terminal Organoimido and Oxo Functional Groups. A New Class of Organo-f-Element Complexes
journal, September 1995

Quantitative Evaluation of Lewis Acidity of Metal Ions with Different Ligands and Counterions in Relation to the Promoting Effects of Lewis Acids on Electron Transfer Reduction of Oxygen
journal, June 2003

Knowledge and Know‐How in Emission Control for Mobile Applications
journal, December 2004

Reactivity of hydrazines with organometallic samarium complexes and the x-ray crystal structures of (C5Me5)2Sm(.eta.2-PhNHNPh)(THF), (C5Me5)2Sm(NHPh)(THF), and [(C5Me5)2Sm]2(.mu.-.eta.2:.eta.2-HNNH)
journal, August 1992

Synthetic, structural, and reactivity studies of the reduction and carbon monoxide derivatization of azobenzene mediated by divalent lanthanide complexes
journal, July 1988

Ceric Ion Oxidation in Organic Chemistry
journal, January 1973

A direct-methane fuel cell with a ceria-based anode
journal, August 1999

A Ligand Field Series for the 4f-Block from Experimental and DFT Computed Ce(IV/III) Electrochemical Potentials
journal, February 2015

Matrix Infrared Spectroscopic and Computational Investigations of the Lanthanide−Methylene Complexes CH ₂ LnF ₂ with Single Ln−C Bonds
journal, March 2011

Lanthanide and Actinide Chemistry
book, January 2006

Unified View of Oxidative C–H Bond Cleavage and Sulfoxidation by a Nonheme Iron(IV)–Oxo Complex via Lewis Acid-Promoted Electron Transfer
journal, March 2014

Development of heterogeneous base catalysts for biodiesel production
journal, June 2008

Studies of the water-gas-shift reaction on ceria-supported Pt, Pd, and Rh: Implications for oxygen-storage properties
journal, January 1998

Iron-Mediated Hydrazine Reduction and the Formation of Iron-Arylimide Heterocubanes
journal, February 2011

Metal Ion-Catalyzed Cycloaddition vs Hydride Transfer Reactions of NADH Analogues with p -Benzoquinones
journal, October 2001

Diamagnetic Corrections and Pascal's Constants
journal, April 2008

Cerium(IV) Trifluoromethanesulfonate as a Strong Oxidizing Agent
journal, August 1990

Activity of CeOx and TiOx Nanoparticles Grown on Au(111) in the Water-Gas Shift Reaction
journal, December 2007

Synthesis and Reactivity of a Ruthenium(III) Bis(anilide) Dimer by Oxidative Addition of an N,N‘-Disubstituted Hydrazine
journal, July 2007

Molecular Structure and Magnetic Properties of Acetato-Bridged Lanthanide(III) Dimers
journal, September 1995

Catalytic Cracking Reaction of Heavy Oil in the Presence of Cerium Oxide Nanoparticles in Supercritical Water
journal, July 2013

Reduction of Hydrazines, Azo and Azoxy Compounds, and Amine N-Oxides with the NiCl2·2H2O–Li–DTBB (cat.) Combination
journal, October 2000

Utilizing the Evans method with a superconducting NMR spectrometer in the undergraduate laboratory
journal, January 1992

Synthesis, structure, and reactivity of homoleptic cerium(IV) and cerium(III) alkoxides
journal, February 1992

Crystal lattice energy and the Madelung constant
journal, May 1970

A series of three-dimensional architectures constructed from lanthanide-substituted polyoxometalosilicates and lanthanide cations or lanthanide–organic complexes as linkers
journal, January 2012

Absorption Anomalies in Ratio and Subtraction FT-IR Spectroscopy
journal, August 1998

Oxidatively pure chiral (salen)Co(III)-X complexes in situ prepared by Lewis acid-promoted electron transfer from chiral (salen)Co(II) to oxygen: Their application in the hydrolytic kinetic resolution of terminal epoxides
journal, June 2007

Variation of electronic transitions and reduction potentials of cerium( iv ) complexes
journal, January 2014

New perspective of electron transfer chemistry
journal, January 2003

400. The determination of the paramagnetic susceptibility of substances in solution by nuclear magnetic resonance
journal, January 1959

Combined Triple and Double Bonds to Uranium: The N≡U═N−H Uranimine Nitride Molecule Prepared in Solid Argon
journal, April 2011

Application of lanthanide reagents in organic synthesis
journal, January 1992

New Paradigm of Electron Transfer Chemistry in Organic Reactions
journal, January 2003

A homoleptic tetravalent cerium silylamide
journal, January 2013

Dearomatization Reactions of N-Heterocycles Mediated by Group 3 Complexes
journal, January 2010

Renewable Hydrogen from Ethanol by Autothermal Reforming
journal, February 2004

Cerium(IV) Ammonium Nitrate as a Catalyst in Organic Synthesis
journal, June 2010

The Impact of Ligand Reorganization on Cerium(III) Oxidation Chemistry
journal, August 2012

The electrochemical behavior of cerium(III/IV) complexes: Thermodynamics, kinetics and applications in synthesis
journal, February 2014

Dimeric Rare-Earth BINOLate Complexes: Activation of 1,4-Benzoquinone through Lewis Acid Promoted Potential Shifts
journal, March 2013

Cerium( iii ) dialkyl dithiocarbamates from [Ce{N(SiMe ₃ ) ₂ } ₃ ] and tetraalkylthiuram disulfides, and [Ce(κ ² -S ₂ CNEt ₂ ) ₄ ] from the Ce ^III precursor; Tb ^III and Nd ^III analogues
journal, January 2004

Reactivity of Organometallic Tantalum Complexes Containing a Bis(phenoxy)amide (ONO) ^3– Ligand with Aryl Azides and 1,2-Diphenylhydrazine
journal, September 2011

Homoleptic Cerium(III) and Cerium(IV) Nitroxide Complexes: Significant Stabilization of the 4+ Oxidation State
journal, September 2013

A short history of SHELX
journal, December 2007

Magnetic Nanoscaled Fe ₃ O ₄ /CeO ₂ Composite as an Efficient Fenton-Like Heterogeneous Catalyst for Degradation of 4-Chlorophenol
journal, September 2012

Synthesis of Tetranuclear, Four-Coordinate Manganese Clusters with “Pinned Butterfly” Geometry Formed by Metal-Mediated N−N Bond Cleavage in Diphenylhydrazine
journal, March 2011

Recent Advances in Synthetic Transformations Mediated by Cerium(IV) Ammonium Nitrate
journal, January 2004

Lanthanide(II)−Alkali Sandwich Complexes with Cation−Arene π Interactions: Synthesis, Structure, and Solvent-Mediated Redox Transformations
journal, April 2011

Quantitative Evaluation of Lewis Acidity of Organotin Compounds and the Catalytic Reactivity in Electron Transfer
journal, October 2001

Infrared Spectra of the η ² -M(NC)-CH ₃ , CH ₃ -MNC, and CH ₂ ═M(H)NC Complexes Prepared by Reactions of Thorium and Uranium Atoms with Acetonitrile
journal, December 2011

Reductive N−N Bond Cleavage of Diphenylhydrazine and Azobenzene Induced by Coordinatively Unsaturated Cp*Fe{N(SiMe ₃ ) ₂ }
journal, June 2006

Stereochemistry of Discrete Eight-Coördination. I. Basic Analysis
journal, April 1963

Factors Governing Oxygen Reduction in Solid Oxide Fuel Cell Cathodes ^†
journal, October 2004

Idealized polytopal forms. Description of real molecules referenced to idealized polygons or polyhedra in geometric reaction path form
journal, March 1974

Catalytic oxidation of water by an oxo-bridged ruthenium dimer
journal, July 1982

Low-temperature water-gas shift reaction over Cu- and Ni-loaded cerium oxide catalysts
journal, August 2000

Cerium (iv) ammonium nitrate (CAN) as a catalyst in tap water: A simple, proficient and green approach for the synthesis of quinoxalines
journal, January 2006

Uncertainties in Scaling Factors for ab Initio Vibrational Frequencies
journal, September 2005

Tuning Reactivity and Electronic Properties through Ligand Reorganization within a Cerium Heterobimetallic Framework
journal, December 2013

Electronic structure and solution behavior of a tris(N,N′-diphenylhydrazido)manganese(iv) propeller complex
journal, January 2012

Reactivity of a Sterically Hindered Fe(II) Thiolate Dimer with Amines and Hydrazines
journal, December 2008

The lattice energies of the alkali halides
journal, February 1956

Active Nonmetallic Au and Pt Species on Ceria-Based Water-Gas Shift Catalysts
journal, August 2003

Structural variation in copper( i ) complexes with pyridylmethylamide ligands: structural analysis with a new four-coordinate geometry index, τ ₄
journal, January 2007

Kinetic and mechanistic aspects of metal ion catalysis in cerium(IV) oxidation
journal, March 2001

Oxidation of substituted hydrazines by superoxide ion: the initiation step for the autoxidation of 1,2-diphenylhydrazine
journal, August 1984

Reduction of Azobenzene by Naphthaleneytterbium: A Tetranuclear Ytterbium(III) Complex Combining 1,2-Diphenylhydrazido(2−) and Phenylimido Ligands
journal, September 1991

Structural Chemistry of Alkali Metal Phenylhyrazides
journal, November 1996

Direct oxidation of hydrocarbons in a solid-oxide fuel cell
journal, March 2000

Molecular polyhedra of high co-ordination number
journal, January 1967

Magnetism of Lanthanides in Molecular Materials with Transition-Metal Ions and Organic Radicals
journal, June 2002

Synthetic Water-Oxidation Catalysts for Artificial Photosynthetic Water Oxidation ^†
journal, February 1997

An isolable, metastable, geometrically unique manganese(iv) trihydrazide complex poised for reactivity
journal, January 2011

Enantioselective Organocatalysis Using SOMO Activation
journal, April 2007

Designing Catalysts for Nitrene Transfer Using Early Transition Metals and Redox-Active Ligands
journal, October 2011

Segmented contraction scheme for small-core lanthanide pseudopotential basis sets
journal, April 2002

Low co-ordination numbers in lanthanide and actinide compounds. Part I. The preparation and characterization of tris{bis(trimethylsilyl)-amido}lanthanides
journal, January 1973