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  • 1.
    Abdel-Magied, Ahmed F.
    et al.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Shatskiy, Andrey
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Liao, Rong-Zhen
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Laine, Tanja M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Arafa, Wael A. A.
    Stockholm University, Faculty of Science, Department of Organic Chemistry. University Fayoum, Egypt.
    Siegbahn, Per E. M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Kärkäs, Markus D.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Åkermark, Bjorn
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Johnston, Eric V.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Chemical and Photochemical Water Oxidation Mediated by an Efficient Single-Site Ruthenium Catalyst2016In: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, Vol. 9, no 24, p. 3448-3456Article in journal (Refereed)
    Abstract [en]

    Water oxidation is a fundamental step in artificial photosynthesis for solar fuels production. In this study, we report a single-site Ru-based water oxidation catalyst, housing a dicarboxylate-benzimidazole ligand, that mediates both chemical and light-driven oxidation of water efficiently under neutral conditions. The importance of the incorporation of the negatively charged ligand framework is manifested in the low redox potentials of the developed complex, which allows water oxidation to be driven by the mild one-electron oxidant [Ru(bpy)(3)](3+) (bpy = 2,2'-bipyridine). Furthermore, combined experimental and DFT studies provide insight into the mechanistic details of the catalytic cycle.

  • 2. Das, Biswanath
    et al.
    Lee, Bao-Lin
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Karlsson, Erik A.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Åkermark, Torbjörn
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Shatskiy, Andrey
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Demeshko, Serhiy
    Liao, Rong-Zhen
    Laine, Tanja M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Haukka, Matti
    Zeglio, Erica
    Abdel-Magied, Ahmed F.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Siegbahn, Per E. M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Meyer, Franc
    Kärkäs, Markus D.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Johnston, Eric V.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Nordlander, Ebbe
    Åkermark, Björn
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Water oxidation catalyzed by molecular di- and nonanuclear Fe complexes: importance of a proper ligand framework2016In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 45, no 34, p. 13289-13293Article in journal (Refereed)
    Abstract [en]

    The synthesis of two molecular iron complexes, a dinuclear iron(III,III) complex and a nonanuclear iron complex, based on the di-nucleating ligand 2,2'-(2-hydroxy-5-methyl-1,3-phenylene)bis(1H-benzo[d]imidazole-4-carboxylic acid) is described. The two iron complexes were found to drive the oxidation of water by the one-electron oxidant [Ru(bpy)(3)](3+).

  • 3.
    Kärkäs, Markus D.
    et al.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Laine, Tanja M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Åkermark, Torbjörn
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Åkermark, Björn
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Molecular Single-site Ruthenium Complexes Containing a Basic Site: The Use of Structure-activity RelationshipsManuscript (preprint) (Other academic)
    Abstract [en]

    A series of single-site ruthenium(III) complexes (2a-d) were synthesized and characterized, and employed in the oxidation of H2O. A linear free-energy relationship study was conducted in order to establish a correlation between the electrochemical properties and the electronic parameters of the introduced substituents in complexes 2a-d.

  • 4.
    Kärkäs, Markus D.
    et al.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Liao, Rong-Zhen
    Laine, Tanja M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Åkermark, Torbjörn
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Ghanem, Shams
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Siegbahn, Per E. M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Åkermark, Björn
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Molecular ruthenium water oxidation catalysts carrying non-innocent ligands: mechanistic insight through structure-activity relationships and quantum chemical calculations2016In: Catalysis Science & Technology, ISSN 2044-4753, E-ISSN 2044-4761, Vol. 6, no 5, p. 1306-1319Article in journal (Refereed)
    Abstract [en]

    Robust catalysts that mediate H2O oxidation are of fundamental importance for the development of novel carbon-neutral energy technologies. Herein we report the synthesis of a group of single-site Ru complexes. Structure-activity studies revealed that the individual steps in the oxidation of H2O depended differently on the electronic properties of the introduced ligand substituents. The mechanistic details associated with these complexes were investigated experimentally along with quantum chemical calculations. It was found that O-O bond formation for the developed Ru complexes proceeds via high-valent Ru-VI species, where the capability of accessing this species is derived from the non-innocent ligand architecture. This cooperative catalytic involvement and the ability of accessing Ru-VI are intriguing and distinguish these Ru catalysts from a majority of previously reported complexes, and might generate unexplored reaction pathways for activation of small molecules such as H2O.

  • 5.
    Kärkäs, Markus D.
    et al.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Åkermark, Torbjörn
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Johnston, Eric V.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Karim, Shams R.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Laine, Tanja M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Lee, Bao-Lin
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Åkermark, Tobias
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Privalov, Timofei
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Åkermark, Björn
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Water Oxidation by Single-Site Ruthenium Complexes: Using Ligands as Redox and Proton Transfer Mediators2012In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 51, no 46, p. 11589-11593Article in journal (Refereed)
  • 6.
    Laine, Tanja M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Development of Ruthenium Catalysts for Water Oxidation2016Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    An increasing global energy demand requires alternative fuel sources. A promising method is artificial photosynthesis. Although, the artificial processes are different from the natural photosynthetic process, the basic principles are the same, i.e. to split water and to convert solar energy into chemical energy. The energy is stored in bonds, which can at a later stage be released upon combustion. The bottleneck in the artificial systems is the water oxidation. The aim of this research has been to develop catalysts for water oxidation that are stable, yet efficient. The molecular catalysts are comprised of organic ligands that ultimately are responsible for the catalyst structure and activity. These ligands are often based on polypyridines or other nitrogen-containing aromatic compounds. This thesis describes the development of molecular ruthenium catalysts and the evaluation of their ability to mediate chemical and photochemical oxidation of water. Previous work from our group has shown that the introduction of negatively charged groups into the ligand frameworks lowers the redox potentials of the metal complexes. This is beneficial as it makes it possible to drive water oxidation with [Ru(bpy)3]3+-type oxidants (bpy = 2,2’-bipyridine), which can be photochemically generated from the corresponding [Ru(bpy)3]2+ complex. Hence, all the designed ligands herein contain negatively charged groups in the coordination site for ruthenium.

    The first part of this thesis describes the development of two mononuclear ruthenium complexes and the evaluation of these for water oxidation. Both complexes displayed low redox potentials, allowing for water oxidation to be driven either chemically or photochemically using the mild one-electron oxidant [Ru(bpy)3]3+.

    The second part is a structure–activity relationship study on several analogues of mononuclear ruthenium complexes. The complexes were active for water oxidation and the redox potentials of the analogues displayed a linear relationship with the Hammet σmeta parameter. It was also found that the complexes form high-valent Ru(VI) species, which are responsible for mediating O–O bond formation.

    The last part of the thesis describes the development of a dinuclear ruthenium complex and the catalytic performance for chemical and photochemical water oxidation. It was found that the complex undergoes O–O bond formation via a bridging peroxide intermediate, i.e. an I2M–type mechanism.

  • 7.
    Laine, Tanja M.
    et al.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Kärkäs, Markus D.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Liao, Rong-Zhen
    Stockholm University, Faculty of Science, Department of Organic Chemistry. Huazhong University of Science & Technology, People's Republic of China.
    Siegbahn, Per E. M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Åkermark, Björn
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    A Dinuclear Ruthenium-Based Water Oxidation Catalyst: Use of Non-Innocent Ligand Frameworks for Promoting Multi-Electron Reactions2015In: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 21, no 28, p. 10039-10048Article in journal (Refereed)
    Abstract [en]

    Insight into how H2O is oxidized to O-2 is envisioned to facilitate the rational design of artificial water oxidation catalysts, which is a vital component in solar-to-fuel conversion schemes. Herein, we report on the mechanistic features associated with a dinuclear Ru-based water oxidation catalyst. The catalytic action of the designed Ru complex was studied by the combined use of high-resolution mass spectrometry, electrochemistry, and quantum chemical calculations. Based on the obtained results, it is suggested that the designed ligand scaffold in Ru complex 1 has a non-innocent behavior, in which metal-ligand cooperation is an important part during the four-electron oxidation of H2O. This feature is vital for the observed catalytic efficiency and highlights that the preparation of catalysts housing non-innocent molecular frameworks could be a general strategy for accessing efficient catalysts for activation of H2O.

  • 8.
    Laine, Tanja M.
    et al.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Kärkäs, Markus D.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Liao, Rong-Zhen
    Stockholm University, Faculty of Science, Department of Organic Chemistry. Huazhong University of Science & Technology, People's Republic of China.
    Åkermark, Torbjörn
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Lee, Bao-Lin
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Karlsson, Erik A.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Siegbahn, Per E. M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Åkermark, Björn
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Efficient photochemical water oxidation by a dinuclear molecular ruthenium complex2015In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 51, no 10, p. 1862-1865Article in journal (Refereed)
    Abstract [en]

    Herein is described the preparation of a dinuclear molecular Ru catalyst for H2O oxidation. The prepared catalyst mediates the photochemical oxidation of H2O with an efficiency comparable to state-of-the-art catalysts.

  • 9.
    Shatskiy, Andrey
    et al.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Lomoth, Reiner
    Abdel-Magied, Ahmed F.
    Stockholm University, Faculty of Science, Department of Organic Chemistry. Nuclear Materials Authority, Egypt.
    Rabten, Wangchuk
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Laine, Tanja M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Chen, Hong
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK). KTH Royal Institute of Technology, Sweden.
    Sun, Junliang
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Andersson, Pher G.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Kärkäs, Markus D.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Johnston, Eric V.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Åkermark, Björn
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Catalyst-solvent interactions in a dinuclear Ru-based water oxidation catalyst2016In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 45, no 47, p. 19024-19033Article in journal (Refereed)
    Abstract [en]

    Photocatalytic water oxidation represents a key process in conversion of solar energy into fuels and can be facilitated by the use of molecular transition metal-based catalysts. A novel straightforward approach for covalent linking of the catalytic units to other moieties is demonstrated by preparation of a dinuclear complex containing two [Ru(pdc)(pic)(3)]-derived units (pdc = 2,6-pyridinedicarboxylate, pic = 4-picoline). The activity of this complex towards chemical and photochemical oxidation of water was evaluated and a detailed insight is given into the interactions between the catalyst and acetonitrile, a common co-solvent employed to increase solubility of water oxidation catalysts. The solvent-induced transformations were studied by electrochemical and spectroscopic techniques and the relevant quantitative parameters were extracted.

  • 10.
    Svengren, Henrik
    et al.
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Hu, Shichao
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Athanassiadis, Ioannis
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Laine, Tanja M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Johnsson, Mats
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    An Oxofluoride Catalyst Comprised of Transition Metals and a Metalloid for Application in Water Oxidation2015In: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 21, no 37, p. 12991-12995Article in journal (Refereed)
    Abstract [en]

    The application of the recently discovered oxofluoride solid solution (CoxNi1-x)(3)Sb4O6F6 as a catalyst for water oxidation is demonstrated. The phase exhibits a cubic arrangement of the active metal that forms oxo bridges to the metalloid with possible catalytic participation. The Co3Sb4O6F6 compound proved to be capable of catalyzing 2H(2)OO(2)+4H(+)+4e(-) at 0.33V electrochemical and 0.39V chemical overpotential with a TOF of 4.410(-3), whereas Ni3Sb4O6F6 needs a higher overpotential. Relatively large crystal cubes (0.3-0.5mm) are easily synthesized and readily handled as they demonstrate both chemical resistance to wear after repeated insitu tests under experimental conditions, and have a mechanical hardness of 270V0.1 using Vickers indentation. The combined properties of this compound offer a potential technical advantage for incorporation to a catalytic interface in future sustainable fuel production.

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