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The Effects of Electron-Donating Substituents on [Ir(bpy)Cp*Cl]+: Water Oxidation versus Ligand Oxidative Modifications

A series of [Ir(bpy)Cp*Cl]Cl (bpy: 2,2'-bipyridine; Cp*: pentamethylcyclopentadienyl) complexes with 4,4'- and 6,6'-substituents on the bipyridine ring were synthesized and used for water oxidation both electrochemically and with chemical oxidants. Under electrochemical water-oxidation reaction (WOR... Full description

Journal Title: European Journal of Inorganic Chemistry Feb 2014, Vol.2014(4), pp.698-707
Main Author: Zhang, Teng
Other Authors: Dekrafft, Kathryn E , Wang, Jin-Liang , Wang, Cheng , Lin, Wenbin
Format: Electronic Article Electronic Article
Language: English
Subjects:
ID: ISSN: 14341948 ; E-ISSN: 10990682 ; DOI: 10.1002/ejic.201300882
Link: http://search.proquest.com/docview/1546001616/?pq-origsite=primo
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title: The Effects of Electron-Donating Substituents on [Ir(bpy)Cp*Cl]+: Water Oxidation versus Ligand Oxidative Modifications
format: Article
creator:
  • Zhang, Teng
  • Dekrafft, Kathryn E
  • Wang, Jin-Liang
  • Wang, Cheng
  • Lin, Wenbin
subjects:
  • Oxidation
  • Ligands
ispartof: European Journal of Inorganic Chemistry, Feb 2014, Vol.2014(4), pp.698-707
description: A series of [Ir(bpy)Cp*Cl]Cl (bpy: 2,2'-bipyridine; Cp*: pentamethylcyclopentadienyl) complexes with 4,4'- and 6,6'-substituents on the bipyridine ring were synthesized and used for water oxidation both electrochemically and with chemical oxidants. Under electrochemical water-oxidation reaction (WOR) conditions at pH = 1, blue films were observed to deposit on the electrode surfaces for all of the complexes, without the detection of oxygen. For chemically driven WORs, three oxidants with different overpotentials and electron-transfer kinetics led to very different behaviors. [Ru(bpy)3]3+ was shown to slowly oxidize the ligands without generating oxygen at pH = 3.7. With NaIO4 as the oxidant at neutral pH, oxygen generation was observed, but ligand oxidation was also seen for the complexes with electron-donating substituents such as -OMe or -OH groups. With Ce4+ as the oxidant at pH = 1, a competition between water oxidation and ligand decomposition existed; less ligand decomposition was...
language: eng
source:
identifier: ISSN: 14341948 ; E-ISSN: 10990682 ; DOI: 10.1002/ejic.201300882
fulltext: fulltext
issn:
  • 14341948
  • 1434-1948
  • 10990682
  • 1099-0682
url: Link


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titleThe Effects of Electron-Donating Substituents on [Ir(bpy)Cp*Cl]+: Water Oxidation versus Ligand Oxidative Modifications
creatorZhang, Teng ; Dekrafft, Kathryn E ; Wang, Jin-Liang ; Wang, Cheng ; Lin, Wenbin
ispartofEuropean Journal of Inorganic Chemistry, Feb 2014, Vol.2014(4), pp.698-707
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descriptionA series of [Ir(bpy)Cp*Cl]Cl (bpy: 2,2'-bipyridine; Cp*: pentamethylcyclopentadienyl) complexes with 4,4'- and 6,6'-substituents on the bipyridine ring were synthesized and used for water oxidation both electrochemically and with chemical oxidants. Under electrochemical water-oxidation reaction (WOR) conditions at pH = 1, blue films were observed to deposit on the electrode surfaces for all of the complexes, without the detection of oxygen. For chemically driven WORs, three oxidants with different overpotentials and electron-transfer kinetics led to very different behaviors. [Ru(bpy)3]3+ was shown to slowly oxidize the ligands without generating oxygen at pH = 3.7. With NaIO4 as the oxidant at neutral pH, oxygen generation was observed, but ligand oxidation was also seen for the complexes with electron-donating substituents such as -OMe or -OH groups. With Ce4+ as the oxidant at pH = 1, a competition between water oxidation and ligand decomposition existed; less ligand decomposition was...
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titleThe Effects of Electron-Donating Substituents on [Ir(bpy)Cp*Cl]+: Water Oxidation versus Ligand Oxidative Modifications
descriptionA series of [Ir(bpy)Cp*Cl]Cl (bpy: 2,2'-bipyridine; Cp*: pentamethylcyclopentadienyl) complexes with 4,4'- and 6,6'-substituents on the bipyridine ring were synthesized and used for water oxidation both electrochemically and with chemical oxidants. Under electrochemical water-oxidation reaction (WOR) conditions at pH = 1, blue films were observed to deposit on the electrode surfaces for all of the complexes, without the detection of oxygen. For chemically driven WORs, three oxidants with different overpotentials and electron-transfer kinetics led to very different behaviors. [Ru(bpy)3]3+ was shown to slowly oxidize the ligands without generating oxygen at pH = 3.7. With NaIO4 as the oxidant at neutral pH, oxygen generation was observed, but ligand oxidation was also seen for the complexes with electron-donating substituents such as -OMe or -OH groups. With Ce4+ as the oxidant at pH = 1, a competition between water oxidation and ligand decomposition existed; less ligand decomposition was...
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abstractA series of [Ir(bpy)Cp*Cl]Cl (bpy: 2,2'-bipyridine; Cp*: pentamethylcyclopentadienyl) complexes with 4,4'- and 6,6'-substituents on the bipyridine ring were synthesized and used for water oxidation both electrochemically and with chemical oxidants. Under electrochemical water-oxidation reaction (WOR) conditions at pH = 1, blue films were observed to deposit on the electrode surfaces for all of the complexes, without the detection of oxygen. For chemically driven WORs, three oxidants with different overpotentials and electron-transfer kinetics led to very different behaviors. [Ru(bpy)3]3+ was shown to slowly oxidize the ligands without generating oxygen at pH = 3.7. With NaIO4 as the oxidant at neutral pH, oxygen generation was observed, but ligand oxidation was also seen for the complexes with electron-donating substituents such as -OMe or -OH groups. With Ce4+ as the oxidant at pH = 1, a competition between water oxidation and ligand decomposition existed; less ligand decomposition was...
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