Photochemical water oxidation by cyclometalated iridium(iii) complexes: a mechanistic insight

2016 ◽  
Vol 52 (19) ◽  
pp. 3840-3843 ◽  
Author(s):  
Sujay Mukhopadhyay ◽  
Roop Shikha Singh ◽  
Arnab Biswas ◽  
Daya Shankar Pandey
Keyword(s):  
Water Oxidation ◽  
Catalytic Cycle ◽  
Mechanistic Insight ◽  
High Valent

Three cyclometalated Ir(iii) complexes for photochemical water oxidation with the realization of high valent iridium in the catalytic cycle are presented.

Mechanistic Insight into the Aromatic Hydroxylation by High-Valent Iron(IV)-oxo Porphyrin π-Cation Radical Complexes

2007 ◽  
Vol 72 (16) ◽  
pp. 6301-6304 ◽  
Author(s):  
Min-Jung Kang ◽  
Woon Ju Song ◽  
Ah-Rim Han ◽  
Young S. Choi ◽  
Ho G. Jang ◽  
...  
Keyword(s):  
Cation Radical ◽  
Mechanistic Insight ◽  
Aromatic Hydroxylation ◽  
High Valent ◽  
Insight Into

scholarly journals Aromaticity Driven Electrocatalytic Water Oxidation by a Phosphorus-Nitrogen PN3-Pincer Cobalt Complex

2019 ◽  
Author(s):  
Pradip K. Das ◽  
Sarmistha Bhunia ◽  
Priyanka Chakraborty ◽  
Atanu Rana ◽  
Abhishek Dey ◽  
...  
Keyword(s):  
Water Oxidation ◽  
High Efficiency ◽  
Cobalt Complex ◽  
Potential Jump ◽  
Onset Potential ◽  
New Strategy ◽  
Earth Abundant ◽  
High Valent ◽  
Lower Overpotential ◽  
Cobalt Species

Water oxidation is the primary step in both natural and artificial photosynthesis to convert solar energy in into chemical fuels. Herein, we report the first cobalt-based pincer catalyst for electrolytic water oxidation at neutral pH with high efficiency under electrochemical conditions. Most importantly, ligand (pseudo)aromaticity is identified to play an important role in the electrocatalysis. A significant potential jump (~300 mV) was achieved towards a lower positive value when the aromatized cobalt complex was transformed to a (pseudo)dearomatized cobalt species. This complex catalyzes the water oxidation in its high valent oxidation state at a much lower overpotential (~ 340 mV vs. NHE) based on the onset potential (0.5 mA/cm<sup>2</sup>) of catalysis at pH 10.5, outperforming all the other literature systems. These observations may provide a new strategy for the design of earth-abundant transition metal-based water oxidation catalysts.

The Catalytic Cycle of Water Oxidation in Crystallized Photosystem II Complexes: Performance and Requirements for Formation of Intermediates

ACS Catalysis ◽  
2019 ◽  
Vol 9 (2) ◽  
pp. 1396-1407 ◽  
Author(s):  
Gennady Ananyev ◽  
Shatabdi Roy-Chowdhury ◽  
Colin Gates ◽  
Petra Fromme ◽  
G. Charles Dismukes
Keyword(s):  
Photosystem Ii ◽  
Water Oxidation ◽  
Catalytic Cycle

Mechanistic Insight into Alcohol Oxidation by High-Valent Iron-Oxo Complexes of Heme and Nonheme Ligands

2005 ◽  
Vol 44 (27) ◽  
pp. 4235-4239 ◽  
Author(s):  
Na Young Oh ◽  
Yumi Suh ◽  
Mi Joo Park ◽  
Mi Sook Seo ◽  
Jinheung Kim ◽  
...  
Keyword(s):  
Alcohol Oxidation ◽  
Oxo Complexes ◽  
Mechanistic Insight ◽  
High Valent ◽  
Insight Into

Tracking the FeIV(O) intermediate and O–O bond formation of a nonheme iron catalyst for water oxidation

2017 ◽  
Vol 53 (65) ◽  
pp. 9063-9066 ◽  
Author(s):  
Bing Yang ◽  
Qing-Qing Yang ◽  
Xin Jiang ◽  
Bin Chen ◽  
Chen-Ho Tung ◽  
...  
Keyword(s):  
Oxygen Evolution ◽  
Water Oxidation ◽  
Iron Catalyst ◽  
Bond Formation ◽  
Nonheme Iron ◽  
High Valent

We describe here a new complex 1 by subtle modulation of the TPA ligand and succeed in capturing the high-valent FeIV(O) species, which is responsible for the O–O bond formation and oxygen evolution with higher efficiency.

Electrocatalytic water oxidation by a molecular cobalt complex through a high valent cobalt oxo intermediate

2016 ◽  
Vol 52 (79) ◽  
pp. 11787-11790 ◽  
Author(s):  
Debasree Das ◽  
Santanu Pattanayak ◽  
Kundan K. Singh ◽  
Bikash Garai ◽  
Sayam Sen Gupta
Keyword(s):  
Water Oxidation ◽  
Cobalt Complex ◽  
High Valent

Biuret-modified tetraamidomacrocyclic cobalt complex [CoIII-bTAML]− is shown to catalyze electrochemical water oxidation at basic pH leading to the formation of O2.

scholarly journals Molecular water oxidation catalysis by zwitterionic carboxylate bridge-functionalized bis-NHC iridium complexes

2019 ◽  
Vol 9 (6) ◽  
pp. 1437-1450 ◽  
Author(s):  
Raquel Puerta-Oteo ◽  
M. Victoria Jiménez ◽  
Jesús J. Pérez-Torrente
Keyword(s):  
Water Oxidation ◽  
Oxidation Catalysis ◽  
Molecular Water ◽  
Iridium Complexes ◽  
Intermediate Species ◽  
Carboxylate Bridge ◽  
Water Oxidation Catalysis ◽  
High Valent

Carboxylate functionalized bis-NHC ligands allow for the stabilization of high-valent iridium intermediate species involved in homogeneous water oxidation catalysis.

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