Mechanisms of molecular water oxidation in solution and on oxide surfaces

Meyer, Thomas J.; Sheridan, Matthew V.; Sherman, Benjamin D.

doi:10.1039/c7cs00465f

Cited by 167 publications

(148 citation statements)

References 99 publications

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“…). However, these attempts can lead to complex synthetic procedures and cause localization, back transfer, and recombination of charge carriers near the photoelectrode/electrolyte interfaces , , …”

Section: Immobilization Of Molecular Electrocatalysts By Covalent mentioning

confidence: 99%

Tailored Assembly of Molecular Water Oxidation Catalysts on Photoelectrodes for Artificial Photosynthesis

et al. 2019

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Solar‐to‐chemical energy conversion, or so‐called artificial photosynthesis, is a promising technology enabling sustainable production and use of various chemical compounds such as H2, CO, CH4, HCOOH, CH3OH, and NH3. For practical applications, it is necessary to improve the interfacial properties of light‐harvesting semiconductors through modification with proper electrocatalysts, by trying to overcome their intrinsic limitations such as rapid recombination, sluggish reaction kinetics, and photocorrosion. Compared to their heterogeneous counterparts, molecular electrocatalysts have a higher catalytic activity and more flexibility in their design/synthesis and integration with semiconducting materials. In this article, we review recent efforts on the tailored assembly of molecular electrocatalysts to address the above issues for artificial photosynthesis, especially those for oxygen evolution reactions on semiconductor photoelectrodes for photoelectrochemical water oxidation. One can expect that the strategies and methods developed for the tailored assembly and integration of molecular electrocatalysts on water oxidation photoanodes can provide insights for the design and fabrication of various forms of photosynthetic devices due to the similarity between their underlying principles.

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Section: Immobilization Of Molecular Electrocatalysts By Covalent mentioning

confidence: 99%

Tailored Assembly of Molecular Water Oxidation Catalysts on Photoelectrodes for Artificial Photosynthesis

et al. 2019

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“…Facilitating such preorganization then led to the development of some of the most potent WOCs to date . Nevertheless, the applicability of these catalysts in complete water splitting cells is limited as they require unrestricted translational mobility, while development of efficient polynuclear WOCs operating via I2M is hampered by the high sensitivity of the mechanism because of geometrical perturbations , …”

Section: Evaluation Of Water Oxidation Catalysts and Mechanistic Consmentioning

confidence: 99%

The Art of Splitting Water: Storing Energy in a Readily Available and Convenient Form

Shatskiy

Kärkäs

2019

Eur J Inorg Chem

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This essay for EurJIC's special issue on “Redox Catalysis for Artificial Photosynthesis” introduces the reader to the field of water oxidation using molecular catalysts. The most essential challenge our society must address during the 21st century is perhaps the realization of a system for producing sustainable energy on the global scale. Currently, there exists an urgent need to develop effective and economical carbon‐neutral or carbon‐free energy technologies. The production of solar fuels through water splitting constitutes a key enabling element. The construction of robust and efficient catalysts for oxidation of water is therefore essential. In this essay the progress and mechanistic considerations pertaining to molecular water oxidation catalysts are described and discussed from a personal perspective.

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“…However, the prevalent detachment of the adsorbed molecular WOCs from the surface of photoanodes during PEC reaction would inevitably result in the poor PEC stability and then greatly impair the water oxidation performance , . To stabilize the molecular WOCs adsorbed on the photoanode surface, atomic layer deposition (ALD) has been explored as one of the most important techniques to coat a stable and ultrathin overlayer onto the photoanode surface to bound molecular complexes and prevent them detaching from the photoanode surface , . It has been well documented that the ALD deposited metal oxide ultrathin layer of TiO 2 or Al 2 O 3 could effectively stabilize the molecular WOCs for PEC water splitting , .…”

Section: Introductionmentioning

confidence: 99%

Protected Hematite Nanorod Arrays with Molecular Complex Co‐Catalyst for Efficient and Stable Photoelectrochemical Water Oxidation

Chen

Kong

et al. 2018

Eur J Inorg Chem

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Herein, a hybrid structure of hematite (α‐Fe2O3) nanorod arrays is designed, with surface catalyzed by Co molecular complex (Co(dca)2, dca: dicyanamide) and then protected by TiO2 thin overlayer, for efficient and stable photoelectrochemical (PEC) water oxidation. The obtained α‐Fe2O3/Co(dca)2/TiO2 hybrid nanorod arrays show much improved and stabilized PEC performance as compared to the pristine, and even the Co(dca)2 or TiO2 modified α‐Fe2O3, with a photocurrent density of 0.35 mA cm–2 obtained at 1.23 V vs. reversible hydrogen electrode (RHE), and an incident photon‐to‐current conversion efficiency (IPCE) reaching 16 % at 400 nm at 1.6 V vs. RHE. It has been demonstrated that the adsorbed Co(dca)2 molecular complex could effectively promote the interface charge transfer process and accelerate the water oxidation reaction kinetics, meanwhile the atomic layer deposited TiO2 overlayer could passivate the surface defects of α‐Fe2O3 and suppress the surface charge carrier recombination. Moreover, the TiO2 overlayer could effectively protect Co(dca)2 from detaching from the α‐Fe2O3 surface and thus stabilize the PEC activity for water oxidation reaction. The present study provides some available thoughts and methods for rational design of highly efficient photoelectrodes for water splitting from the perspective of the surface and interface engineered charge carrier transfer and water oxidation processes.

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Mechanisms of molecular water oxidation in solution and on oxide surfaces

Cited by 167 publications

References 99 publications

Tailored Assembly of Molecular Water Oxidation Catalysts on Photoelectrodes for Artificial Photosynthesis

Tailored Assembly of Molecular Water Oxidation Catalysts on Photoelectrodes for Artificial Photosynthesis

The Art of Splitting Water: Storing Energy in a Readily Available and Convenient Form

Protected Hematite Nanorod Arrays with Molecular Complex Co‐Catalyst for Efficient and Stable Photoelectrochemical Water Oxidation

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