Special Issue "Water Oxidation Catalysis"

A special issue of Catalysts (ISSN 2073-4344).

Deadline for manuscript submissions: closed (30 November 2017).

Special Issue Editor

Guest Editor
Dr. Yurii V. Geletii

Department of Chemistry, Emory University, Atlanta, GA 30322, USA
Website | E-Mail
Interests: artificial photosynthesis; water splitting; water oxidation catalysts; electron transfer reactions

Special Issue Information

Dear Colleagues,

Almost all life on Earth relies directly, or indirectly, on solar light as a source of energy. Nature has created a very complex system, Photosynthesis, to convert light energy to biomass and oxygen. However, the low efficiency of Photosynthesis rules out the use of biomass as the main source of energy for modern civilization. The use of sunlight to split water into dioxygen and hydrogen (the basic initial fuel) could be a vast, inexhaustible, and clean source of energy. The efficiency of this impressive method to split water depends on the efficiency of water oxidation and water reduction catalysts. The main focus of this Special Issue on “Water Oxidation Catalysis” will be on molecular Water Oxidation Catalysts (WOC). Original research papers and short reviews on synthesis, characterization of new catalysts, studies of activity and stability of molecular complexes under turnover conditions,  identification of intermediates in the catalytic cycle, the mechanisms of O–O formation, and the role of protons, cations, and anions on electron transfer reactions in water oxidation, are invited for submission.  

Dr. Yurii V. Geletii
Guest Editor

Manuscript Submission Information

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Keywords

  • water splitting
  • molecular water oxidation catalysts
  • activity and stability of WOC
  • kinetics of water oxidation reactions
  • intermediates in water oxidation catalytic cycle
  • electron transfer reactions in water oxidation catalytic cycle
  • mechanism of O–O bond formation

Published Papers (4 papers)

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Research

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Open AccessCommunication
Enzymatic Oxyfunctionalization Driven by Photosynthetic Water-Splitting in the Cyanobacterium Synechocystis sp. PCC 6803
Catalysts 2017, 7(8), 240; https://doi.org/10.3390/catal7080240
Received: 8 July 2017 / Revised: 10 August 2017 / Accepted: 10 August 2017 / Published: 17 August 2017
Cited by 7 | PDF Full-text (1274 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
Photosynthetic water-splitting is a powerful force to drive selective redox reactions. The need of highly expensive redox partners such as NADPH and their regeneration is one of the main bottlenecks for the application of biocatalysis at an industrial scale. Recently, the possibility of [...] Read more.
Photosynthetic water-splitting is a powerful force to drive selective redox reactions. The need of highly expensive redox partners such as NADPH and their regeneration is one of the main bottlenecks for the application of biocatalysis at an industrial scale. Recently, the possibility of using the photosystem of cyanobacteria to supply high amounts of reduced nicotinamide to a recombinant enoate reductase opened a new strategy for overcoming this hurdle. This paper presents the expansion of the photosynthetic regeneration system to a Baeyer–Villiger monooxygenase. Despite the potential of this strategy, this work also presents some of the encountered challenges as well as possible solutions, which will require further investigation. The successful enzymatic oxygenation shows that cyanobacterial whole-cell biocatalysis is an applicable approach that allows fuelling selective oxyfunctionalisation reactions at the expense of light and water. Yet, several hurdles such as side-reactions and the cell-density limitation, probably due to self-shading of the cells, will have to be overcome on the way to synthetic applications. Full article
(This article belongs to the Special Issue Water Oxidation Catalysis)
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Open AccessArticle
Mechanism of Water Oxidation Catalyzed by a Dinuclear Ruthenium Complex Bridged by Anthraquinone
Catalysts 2017, 7(2), 56; https://doi.org/10.3390/catal7020056
Received: 5 January 2017 / Revised: 2 February 2017 / Accepted: 6 February 2017 / Published: 10 February 2017
Cited by 4 | PDF Full-text (3982 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
We synthesized 1,8-bis(2,2′:6′,2″-terpyrid-4′-yl)anthraquinone (btpyaq) as a new dimerizing ligand and determined its single crystal structure by X-ray analysis. The dinuclear Ruthenium complex [Ru2(µ-Cl)(bpy)2(btpyaq)](BF4)3 ([3](BF4)3, bpy = 2,2′-bipyridine) was used as a catalyst for water oxidation to oxygen with (NH4)2[Ce(NO3)6] as the oxidant (turnover [...] Read more.
We synthesized 1,8-bis(2,2′:6′,2″-terpyrid-4′-yl)anthraquinone (btpyaq) as a new dimerizing ligand and determined its single crystal structure by X-ray analysis. The dinuclear Ruthenium complex [Ru2(µ-Cl)(bpy)2(btpyaq)](BF4)3 ([3](BF4)3, bpy = 2,2′-bipyridine) was used as a catalyst for water oxidation to oxygen with (NH4)2[Ce(NO3)6] as the oxidant (turnover numbers = 248). The initial reaction rate of oxygen evolution was directly proportional to the concentration of the catalyst and independent of the oxidant concentration. The cyclic voltammogram of [3](BF4)3 in water at pH 1.3 showed an irreversible catalytic current above +1.6 V (vs. SCE), with two quasi-reversible waves and one irreversible wave at E1/2 = +0.62, +0.82 V, and Epa = +1.13 V, respectively. UV-vis and Raman spectra of [3](BF4)3 with controlled-potential electrolysis at +1.40 V revealed that [Ru(IV)=O O=Ru(IV)]4+ is stable under electrolysis conditions. [Ru(III), Ru(II)] species are recovered after dissociation of an oxygen molecule from the active species in the catalytic cycle. These results clearly indicate that an O–O bond is formed via [Ru(V)=O O=Ru(IV)]5+. Full article
(This article belongs to the Special Issue Water Oxidation Catalysis)
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Review

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Open AccessReview
Photocatalytic Water Oxidation on ZnO: A Review
Catalysts 2017, 7(3), 93; https://doi.org/10.3390/catal7030093
Received: 16 December 2016 / Revised: 27 February 2017 / Accepted: 2 March 2017 / Published: 21 March 2017
Cited by 32 | PDF Full-text (239 KB) | HTML Full-text | XML Full-text
Abstract
The investigation of the water oxidation mechanism on photocatalytic semiconductor surfaces has gained much attention for its potential to unlock the technological limitations of producing H2 from carbon-free sources, i.e., H2O. This review seeks to highlight the available scientific and [...] Read more.
The investigation of the water oxidation mechanism on photocatalytic semiconductor surfaces has gained much attention for its potential to unlock the technological limitations of producing H2 from carbon-free sources, i.e., H2O. This review seeks to highlight the available scientific and fundamental understanding towards the water oxidation mechanism on ZnO surfaces, as well as present a summary on the modification strategies carried out to increase the photocatalytic response of ZnO. Full article
(This article belongs to the Special Issue Water Oxidation Catalysis)
Open AccessFeature PaperReview
Recent Advances in the BiVO4 Photocatalyst for Sun-Driven Water Oxidation: Top-Performing Photoanodes and Scale-Up Challenges
Catalysts 2017, 7(1), 13; https://doi.org/10.3390/catal7010013
Received: 24 November 2016 / Revised: 28 December 2016 / Accepted: 28 December 2016 / Published: 1 January 2017
Cited by 70 | PDF Full-text (5521 KB) | HTML Full-text | XML Full-text
Abstract
Photoelectrochemical (PEC) water splitting, which is a type of artificial photosynthesis, is a sustainable way of converting solar energy into chemical energy. The water oxidation half-reaction has always represented the bottleneck of this process because of the thermodynamic and kinetic challenges that are [...] Read more.
Photoelectrochemical (PEC) water splitting, which is a type of artificial photosynthesis, is a sustainable way of converting solar energy into chemical energy. The water oxidation half-reaction has always represented the bottleneck of this process because of the thermodynamic and kinetic challenges that are involved. Several materials have been explored and studied to address the issues pertaining to solar water oxidation. Significant advances have recently been made in the use of stable and relatively cheap metal oxides, i.e., semiconducting photocatalysts. The use of BiVO4 for this purpose can be considered advantageous because this catalyst is able to absorb a substantial portion of the solar spectrum and has favourable conduction and valence band edge positions. However, BiVO4 is also associated with poor electron mobility and slow water oxidation kinetics and these are the problems that are currently being investigated in the ongoing research in this field. This review focuses on the most recent advances in the best-performing BiVO4-based photoanodes to date. It summarizes the critical parameters that contribute to the performance of these photoanodes, and highlights so far unresolved critical features related to the scale-up of a BiVO4-based PEC water-splitting device. Full article
(This article belongs to the Special Issue Water Oxidation Catalysis)
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