Highly efficient and robust molecular ruthenium catalysts for water oxidation.
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TLDR
Aiming at developing robust molecular Ru-bda (H2bda = 2,2′-bipyridine-6,6′-dicarboxylic acid) water oxidation catalysts, density functional theory studies were carried out, the robustness of catalysts against hydration was correlated with the highest occupied molecular orbital levels of a set of ligands, and the synthesis of robust Ru(bda)L2 was directed.Abstract:
Water oxidation catalysts are essential components of light-driven water splitting systems, which could convert water to H2 driven by solar radiation (H2O + hν → 1/2O2 + H2). The oxidation of water (H2O → 1/2O2 + 2H+ + 2e-) provides protons and electrons for the production of dihydrogen (2H+ + 2e- → H2), a clean-burning and high-capacity energy carrier. One of the obstacles now is the lack of effective and robust water oxidation catalysts. Aiming at developing robust molecular Ru-bda (H2bda = 2,2′-bipyridine-6,6′-dicarboxylic acid) water oxidation catalysts, we carried out density functional theory studies, correlated the robustness of catalysts against hydration with the highest occupied molecular orbital levels of a set of ligands, and successfully directed the synthesis of robust Ru-bda water oxidation catalysts. A series of mononuclear ruthenium complexes [Ru(bda)L2] (L = pyridazine, pyrimidine, and phthalazine) were subsequently synthesized and shown to effectively catalyze CeIV-driven [CeIV = Ce(NH4)2(NO3)6] water oxidation with high oxygen production rates up to 286 s-1 and high turnover numbers up to 55,400.read more
Citations
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Artificial photosynthesis: molecular systems for catalytic water oxidation.
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Chemical approaches to artificial photosynthesis
TL;DR: In the early 1970s, the works by Fujishima and Honda (1) and Honda et al. (2) reported on the results of a now famous experiment that showed that band gap excitation of anatase TiO2 in a photoelectrochemical cell with a Pt counter electrode and an applied bias resulted in water splitting into hydrogen and oxygen.
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Molecular Chromophore–Catalyst Assemblies for Solar Fuel Applications
Dennis L. Ashford,Melissa K. Gish,Aaron K. Vannucci,M. Kyle Brennaman,Joseph L. Templeton,John M. Papanikolas,Thomas J. Meyer +6 more
TL;DR: Applications Dennis L. Ashford,† Melissa K. Gish,† Aaron K. Vannucci,‡ M. Kyle Brennaman,† Joseph L. Templeton,† John M. Papanikolas,† and Thomas J. Meyer are submitted.
References
More filters
Journal ArticleDOI
Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density
TL;DR: Numerical calculations on a number of atoms, positive ions, and molecules, of both open- and closed-shell type, show that density-functional formulas for the correlation energy and correlation potential give correlation energies within a few percent.
Journal ArticleDOI
The M06 suite of density functionals for main group thermochemistry, thermochemical kinetics, noncovalent interactions, excited states, and transition elements: two new functionals and systematic testing of four M06-class functionals and 12 other functionals
Yan Zhao,Donald G. Truhlar +1 more
TL;DR: The M06-2X meta-exchange correlation function is proposed in this paper, which is parametrized including both transition metals and nonmetals, and is a high-non-locality functional with double the amount of nonlocal exchange.
Journal ArticleDOI
A Fast Soluble Carbon-Free Molecular Water Oxidation Catalyst Based on Abundant Metals
Qiushi Yin,Jeffrey Miles Tan,Claire Besson,Claire Besson,Yurii V. Geletii,Djamaladdin G. Musaev,Aleksey E. Kuznetsov,Zhen Luo,Ken I. Hardcastle,Craig L. Hill +9 more
TL;DR: Extensive spectroscopic, electrochemical, and inhibition studies firmly indicate that [Co4(H2O)2(PW9O34)2]10– is stable under catalytic turnover conditions: Neither hydrated cobalt ions nor cobalt hydroxide/oxide particles form in situ.
Journal ArticleDOI
Correlation consistent valence basis sets for use with the Stuttgart–Dresden–Bonn relativistic effective core potentials: The atoms Ga–Kr and In–Xe
TL;DR: In this article, the SDB-cc-pVQZ pseudopotential basis set was optimized for use with the large core (valence-electrons only) Stuttgart-Dresden-Bonn relativistic pseudopotentials.
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A molecular ruthenium catalyst with water-oxidation activity comparable to that of photosystem II
Lele Duan,Fernando Bozoglian,Sukanta Mandal,Beverly Stewart,Timofei Privalov,Antoni Llobet,Licheng Sun,Licheng Sun +7 more
TL;DR: It is shown that it is possible to close that 'two orders of magnitude' gap in the efficiency of the water oxidation with a rationally designed molecular catalyst [Ru(bda)(isoq)(2)] (H(2)bda = 2,2'-bipyridine-6,6'-dicarboxylic acid; isoq = isoquinoline).