Einkernige Katalysatoren zur Wasseroxidation

Hetterscheid, Dennis G. H.; Reek, Joost N. H.

doi:10.1002/ange.201202948

Cited by 35 publications

(2 citation statements)

References 83 publications

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“…Understanding the reaction mechanism and identification of the reactive intermediates will give the opportunity for precise catalyst design and also tuning of the active catalysts. [52][53][54][55][56][57][58][59][60][61][62][63][64][65][66][67] According to Oswald's original definitions of homogeneous and heterogeneous catalysis, homogeneous catalysis is one where catalyst and substrate exists in the same phase (i.e. solution) and heterogeneous catalysis is one where catalyst and substrate exists in different phases.…”

Section: Introductionmentioning

confidence: 99%

Earth-abundant metal complexes as catalysts for water oxidation; is it homogeneous or heterogeneous?

Asraf

Younus

Yusubov

et al. 2015

Catal. Sci. Technol.

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MINIREVIEW This journal isRecent developments in the oxidation of water to dioxygen using metal complexes as catalysts or precatalysts are represented at the side of the conversion of homogeneous catalysts into nanoparticles or heterogeneous one during the oxidation reaction of water. Homogeneous catalysts are advantageous within the careful design and elucidation of the mechanisms for the catalytic water oxidation. In distinction, the uses of heterogeneous catalysts in water oxidation are advantageous for sensible applications as a result of their robust catalytic activity. Though detailed studies on homogeneous and heterogeneous water oxidation reactions are performed rather severally, the connection of homogeneous catalysts with heterogeneous one is changing into an additional requirement for the event of economic attractive water oxidation catalysts (WOCs). This minireview focuses on the aspects if the particular catalysts for the oxidation of water are homogeneous or heterogeneous.

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Section: Introductionmentioning

confidence: 99%

Earth-abundant metal complexes as catalysts for water oxidation; is it homogeneous or heterogeneous?

Asraf

Younus

Yusubov

et al. 2015

Catal. Sci. Technol.

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“…In this context the storage of renewable energy into chemical fuels, such as hydrogen, is important [1–5] . Hydrogen can be generated by water electrolysis using sustainable energy, and this reaction is therefore a topic of much recent interest [6–18] . Water electrolysis consists of two half reactions: proton reduction and water oxidation.…”

Section: Methodsmentioning

confidence: 99%

Potential‐ and Buffer‐Dependent Catalyst Decomposition during Nickel‐Based Water Oxidation Catalysis

Hessels

Detz

et al. 2020

ChemSusChem

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The production of hydrogen by water electrolysis benefits from the development of water oxidation catalysts. This development process can be aided by the postulation of design rules for catalytic systems. The analysis of the reactivity of molecular complexes can be complicated by their decomposition under catalytic conditions into nanoparticles that may also be active. Such a misinterpretation can lead to incorrect design rules. In this study, the nickel‐based water oxidation catalyst [NiII(meso‐L)](ClO4)2, which was previously thought to operate as a molecular catalyst, is found to decompose to form a NiOx layer in a pH 7.0 phosphate buffer under prolonged catalytic conditions, as indicated by controlled potential electrolysis, electrochemical quartz crystal microbalance, and X‐ray photoelectron spectroscopy measurements. Interestingly, the formed NiOx layer desorbs from the surface of the electrode under less anodic potentials. Therefore, no nickel species can be detected on the electrode after electrolysis. Catalyst decomposition is strongly dependent on the pH and buffer, as there is no indication of NiOx layer formation at pH 6.5 in phosphate buffer nor in a pH 7.0 acetate buffer. Under these conditions, the activity stems from a molecular species, but currents are much lower. This study demonstrates the importance of in situ characterization methods for catalyst decomposition and metal oxide layer formation, and previously proposed design elements for nickel‐based catalysts need to be revised.

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A Self‐Improved Water‐Oxidation Catalyst: Is One Site Really Enough?

et al. 2013

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The homogeneous catalysis of water oxidation by transition-metal complexes has experienced spectacular development over the last five years. Practical energy-conversion schemes, however, require robust catalysts with large turnover frequencies. Herein we introduce a new oxidatively rugged and powerful dinuclear water-oxidation catalyst that is generated by self-assembly from a mononuclear catalyst during the catalytic process. Our kinetic and DFT computational analysis shows that two interconnected catalytic cycles coexist while the mononuclear system is slowly and irreversibly converted into the more stable dinuclear system: an extremely robust wateroxidation catalyst that does not decompose over extended periods of time.

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Einkernige Katalysatoren zur Wasseroxidation

Cited by 35 publications

References 83 publications

Earth-abundant metal complexes as catalysts for water oxidation; is it homogeneous or heterogeneous?

Earth-abundant metal complexes as catalysts for water oxidation; is it homogeneous or heterogeneous?

Potential‐ and Buffer‐Dependent Catalyst Decomposition during Nickel‐Based Water Oxidation Catalysis

A Self‐Improved Water‐Oxidation Catalyst: Is One Site Really Enough?

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