Multielectron Redox Chemistry of Transition Metal Complexes Supported by a Non-Innocent N3P2 Ligand: Synthesis, Characterization, and Catalytic Properties
Abstract
A new redox‐active, diarylamido‐based ligand ( L N3P2 ) capable of κ 5 ‐ N , N , N,P,P chelation has been used to prepare a series of complexes with the general formula [M II ( L N3P2 )]X, where M = Fe ( 1 ; X = OTf), Co ( 2 ; X = ClO 4 ), or Ni ( 3 ; X = ClO 4 ). The diarylamido core of monoanionic L N3P2 is derived from bis(2‐amino‐4‐methylphenyl)amine, which undergoes condensation with two equivalents of 2‐(diphenylphosphanyl)benzaldehyde to provide chelating arms with both arylphosphine and imine donors. X‐ray structural, magnetic, and spectroscopic studies indicate that the N 3 P 2 coordination environment generally promotes low‐spin configurations. Three quasi‐reversible redox couples between +1.0 and –1.5 V (vs. Fc + /Fc) were observed in voltammetric studies of each complex, corresponding to M II /M III oxidation, L N3P2 ‐based oxidation, and M II /M I reduction (in order of highest to lowest potential). Spectroscopic and computational analyses of 3 ox – generated via chemical one‐electron oxidation of 3 – revealed that a stable diarylaminyl radical ( L N3P2· ) is formed upon oxidation. The ability of the Co II complex ( 2more »
- Authors:
-
[2];
[1]
- Marquette Univ., Milwaukee, WI (United States)
- Wayne State Univ., Detroit, MI (United States)
- Publication Date:
- Research Org.:
- Wayne State Univ., Detroit, MI (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1610585
- Alternate Identifier(s):
- OSTI ID: 1473739
- Grant/Contract Number:
- SC0001907
- Resource Type:
- Accepted Manuscript
- Journal Name:
- European Journal of Inorganic Chemistry
- Additional Journal Information:
- Journal Volume: 2018; Journal Issue: 37; Journal ID: ISSN 1434-1948
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry
Citation Formats
Wang, Denan, Ekanayake, Danushka M., Lindeman, Sergey V., Verani, Cláudio N., and Fiedler, Adam T. Multielectron Redox Chemistry of Transition Metal Complexes Supported by a Non-Innocent N3P2 Ligand: Synthesis, Characterization, and Catalytic Properties. United States: N. p., 2018.
Web. doi:10.1002/ejic.201800843.
Wang, Denan, Ekanayake, Danushka M., Lindeman, Sergey V., Verani, Cláudio N., & Fiedler, Adam T. Multielectron Redox Chemistry of Transition Metal Complexes Supported by a Non-Innocent N3P2 Ligand: Synthesis, Characterization, and Catalytic Properties. United States. https://doi.org/10.1002/ejic.201800843
Wang, Denan, Ekanayake, Danushka M., Lindeman, Sergey V., Verani, Cláudio N., and Fiedler, Adam T. Tue .
"Multielectron Redox Chemistry of Transition Metal Complexes Supported by a Non-Innocent N3P2 Ligand: Synthesis, Characterization, and Catalytic Properties". United States. https://doi.org/10.1002/ejic.201800843. https://www.osti.gov/servlets/purl/1610585.
@article{osti_1610585,
title = {Multielectron Redox Chemistry of Transition Metal Complexes Supported by a Non-Innocent N3P2 Ligand: Synthesis, Characterization, and Catalytic Properties},
author = {Wang, Denan and Ekanayake, Danushka M. and Lindeman, Sergey V. and Verani, Cláudio N. and Fiedler, Adam T.},
abstractNote = {A new redox‐active, diarylamido‐based ligand ( L N3P2 ) capable of κ 5 ‐ N , N , N,P,P chelation has been used to prepare a series of complexes with the general formula [M II ( L N3P2 )]X, where M = Fe ( 1 ; X = OTf), Co ( 2 ; X = ClO 4 ), or Ni ( 3 ; X = ClO 4 ). The diarylamido core of monoanionic L N3P2 is derived from bis(2‐amino‐4‐methylphenyl)amine, which undergoes condensation with two equivalents of 2‐(diphenylphosphanyl)benzaldehyde to provide chelating arms with both arylphosphine and imine donors. X‐ray structural, magnetic, and spectroscopic studies indicate that the N 3 P 2 coordination environment generally promotes low‐spin configurations. Three quasi‐reversible redox couples between +1.0 and –1.5 V (vs. Fc + /Fc) were observed in voltammetric studies of each complex, corresponding to M II /M III oxidation, L N3P2 ‐based oxidation, and M II /M I reduction (in order of highest to lowest potential). Spectroscopic and computational analyses of 3 ox – generated via chemical one‐electron oxidation of 3 – revealed that a stable diarylaminyl radical ( L N3P2· ) is formed upon oxidation. The ability of the Co II complex ( 2 ) to function as an electrocatalyst for H 2 generation was evaluated in the presence of weak acids. Moderate activity was observed using 4‐ tert ‐butylphenol as the proton source at potentials below –2.0 V. The insights gained here will assist in the future design of pentadentate mixed N/P‐based chelates for catalytic processes.},
doi = {10.1002/ejic.201800843},
journal = {European Journal of Inorganic Chemistry},
number = 37,
volume = 2018,
place = {United States},
year = {Tue Sep 25 00:00:00 EDT 2018},
month = {Tue Sep 25 00:00:00 EDT 2018}
}
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Electrocatalytic Reduction of CO2 Using the Complexes [Re(bpy)(CO)3L]n (n = +1, L = P(OEt)3, CH3CN; n = 0, L = Cl-, Otf-; bpy = 2,2‘-Bipyridine; Otf- = CF3SO3) as Catalyst Precursors: Infrared Spectroelectrochemical Investigation
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- Johnson, Frank P. A.; George, Michael W.; Hartl, Frantisek
- Organometallics, Vol. 15, Issue 15
Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density
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- The University of North Carolina at Chapel Hill University Libraries