Catalytic Water Oxidation by a Bio-inspired Nickel Complex with a Redox-Active Ligand

Wang, Dong; Bruner, Charlie O.

doi:10.1021/acs.inorgchem.7b02166

Cited by 68 publications

(65 citation statements)

References 29 publications

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“…, and 2-((bis(pyridin-2ylmethyl)amino)methyl)phenol, have been synthesized and used to assess the performance of catalytic water oxidation. 254,[257][258][259] Some other Ni-based complexes were reported as precursors to generate active Ni oxide films for water oxidation. [260][261][262] Because of the fewer redox states of Ni ions, development of Ni-based WOCs with low overpotentials remains challenging.…”

Section: Overview Of Molecular Water-oxidation Catalysts (Wocs)mentioning

confidence: 99%

Artificial photosynthesis: opportunities and challenges of molecular catalysts

2019

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Section: Overview Of Molecular Water-oxidation Catalysts (Wocs)mentioning

confidence: 99%

Artificial photosynthesis: opportunities and challenges of molecular catalysts

2019

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“…The catalytic current, i c ,i sg iven by Equation (20), which does not dependo nt he scan rate. [85][86][87][88][89]…”

Section: The Third Wave Co V/ivmentioning

confidence: 99%

Cobalt Carbonate as an Electrocatalyst for Water Oxidation

Patra

Illés

Mizrahi³

et al. 2019

Chemistry A European J

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Co II salts in the presence of HCO 3 À /CO 3 2À in aqueous solutionsa ct as electrocatalysts for water oxidation. It comprises of several key steps:( i) Ar elatively small wave at E pa % 0.71 V( vs. Ag/AgCl) owing to the Co III/II redox couple. (ii)Asecond wave is observed at E pa % 1.10 Vwith aconsiderably larger current.I nw hich the Co III undergoes oxidation to form aC o IV species. The large current is attributed to catalytic oxidation of HCO 3 À /CO 3 2À to HCO 4 À .( iii)A process with very large currents at > 1.2 Vo wing to the formation of Co V (CO 3 ) 3 À ,w hich oxidizes both water and HCO 3 À /CO 3 2À . Thesep rocesses depend on [Co II ], [NaHCO 3 ], andp H. Chronoamperometry at 1.3 Vg ives ag reen deposit. It acts as a heterogeneous catalystf or water oxidation. DFT calculations point out that Co n (CO 3 ) 3 nÀ6, n = 4, 5a re attainable at potentials similar to those experimentally observed.Scheme1.Outline of the water oxidation mechanisms. Misthe metal, n represents the highest oxidation state. [50] This figure has beenr eproduced (modified) from reference [50] with permission from the Royal Societyof Chemistry.

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“…[18][19][20][21] True homogeneous catalysis based on Ni complexes are rare and thus is a relatively unexplored field. [22][23][24] In order to decipher the narrow line between homogeneous and heterogeneous catalysis using molecular Ni complexes, we have chosen the recently reported [(L 1 )Ni II ] 2-(L 1 = ophenylenebis(oxamidate)) complex, 1 2-, 19 and its aryl substituted analogues [(L 2 )Ni II ] 2-(L 2 = 4,5-dimethyl-1,2-phenylenebis(oxamidate)), 2 2-, and [(L 3 )Ni II ] 2-(L 2 = 4-methoxy-1,2phenylenebis(oxamidate)), 3 2reported here for the first time (See Figure 1 for a drawn structure and crystal structure). We study in depth the catalytic pathways available to this family of complexes together with the deactivation paths that can lead to the formation of NiOx.…”

Section: Introductionmentioning

confidence: 99%

Can Ni Complexes Behave as Molecular Water Oxidation Catalysts?

et al. 2019

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The present report uncovers the borderline between homogeneous and heterogeneous water oxidation catalysis using a family of Ni complexes containing oxamidate anionic type of ligands. In particular, the Ni complex [(L 1)Ni II ] 2-(1 2-; L 1 = o-phenylenebis(oxamidate)) and its modified analogues [(L 2)Ni II ] 2-(2 2-;L 2 = 4,5-dimethyl-1,2-phenylenebis(oxamidate)) and [(L 3)Ni II ] 2-(3 2-;L 2 = 4methoxy-1,2-phenylenebis(oxamidate)) have been prepared and evaluated as molecular water oxidation catalysts at basic pH. Their redox features have been analyzed by mean of electrochemical measurements revealing a crucial involvement of the ligand in the electron transfer processes. Moreover, the stability of those complexes has been assessed both in solution and immobilized on graphene-based electrodes at different potentials and pHs. The degradation of the molecular species generates a NiOx layer, whose stability and activity as water oxidation catalyst has also been stablished. Electrochemical methods, together with surface characterization techniques, have shown the complex mechanistic scenario in water oxidation catalyzed by this family of Ni complexes, which consists of the coexistence of two catalytic mechanism: a homogeneous pathway driven by the molecular complex and a heterogeneous pathway based on NiOx. The electronic perturbations exerted through the ligand framework has manifested a strong influence over the stability of the molecular species under turnover conditions. Finally, 1 2has been used as a molecular precursor for the formation of NiFeOx anodes that behave as extremely powerful water oxidation anodes.

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Catalytic Water Oxidation by a Bio-inspired Nickel Complex with a Redox-Active Ligand

Cited by 68 publications

References 29 publications

Artificial photosynthesis: opportunities and challenges of molecular catalysts

Artificial photosynthesis: opportunities and challenges of molecular catalysts

Cobalt Carbonate as an Electrocatalyst for Water Oxidation

Can Ni Complexes Behave as Molecular Water Oxidation Catalysts?

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