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  • 1.
    Abdel-Magied, Ahmed F.
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Shatskiy, Andrey
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Liao, Rong-Zhen
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Laine, Tanja M.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Arafa, Wael A. A.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi. University Fayoum, Egypt.
    Siegbahn, Per E. M.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Kärkäs, Markus D.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Åkermark, Bjorn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Johnston, Eric V.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Chemical and Photochemical Water Oxidation Mediated by an Efficient Single-Site Ruthenium Catalyst2016Inngår i: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, Vol. 9, nr 24, s. 3448-3456Artikkel i tidsskrift (Fagfellevurdert)
    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
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Karlsson, Erik A.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Åkermark, Torbjörn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Shatskiy, Andrey
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Demeshko, Serhiy
    Liao, Rong-Zhen
    Laine, Tanja M.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Haukka, Matti
    Zeglio, Erica
    Abdel-Magied, Ahmed F.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Siegbahn, Per E. M.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Meyer, Franc
    Kärkäs, Markus D.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Johnston, Eric V.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Nordlander, Ebbe
    Åkermark, Björn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Water oxidation catalyzed by molecular di- and nonanuclear Fe complexes: importance of a proper ligand framework2016Inngår i: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 45, nr 34, s. 13289-13293Artikkel i tidsskrift (Fagfellevurdert)
    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.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Laine, Tanja M.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Åkermark, Torbjörn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Åkermark, Björn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Molecular Single-site Ruthenium Complexes Containing a Basic Site: The Use of Structure-activity RelationshipsManuskript (preprint) (Annet vitenskapelig)
    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.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Liao, Rong-Zhen
    Laine, Tanja M.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Åkermark, Torbjörn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Ghanem, Shams
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Siegbahn, Per E. M.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Åkermark, Björn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Molecular ruthenium water oxidation catalysts carrying non-innocent ligands: mechanistic insight through structure-activity relationships and quantum chemical calculations2016Inngår i: Catalysis Science & Technology, ISSN 2044-4753, E-ISSN 2044-4761, Vol. 6, nr 5, s. 1306-1319Artikkel i tidsskrift (Fagfellevurdert)
    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.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Åkermark, Torbjörn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Johnston, Eric V.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Karim, Shams R.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Laine, Tanja M.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Lee, Bao-Lin
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Åkermark, Tobias
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Privalov, Timofei
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Åkermark, Björn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Water Oxidation by Single-Site Ruthenium Complexes: Using Ligands as Redox and Proton Transfer Mediators2012Inngår i: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 51, nr 46, s. 11589-11593Artikkel i tidsskrift (Fagfellevurdert)
  • 6.
    Laine, Tanja M.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Development of Ruthenium Catalysts for Water Oxidation2016Doktoravhandling, med artikler (Annet vitenskapelig)
    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.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Kärkäs, Markus D.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Liao, Rong-Zhen
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi. Huazhong University of Science & Technology, People's Republic of China.
    Siegbahn, Per E. M.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Åkermark, Björn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    A Dinuclear Ruthenium-Based Water Oxidation Catalyst: Use of Non-Innocent Ligand Frameworks for Promoting Multi-Electron Reactions2015Inngår i: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 21, nr 28, s. 10039-10048Artikkel i tidsskrift (Fagfellevurdert)
    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.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Kärkäs, Markus D.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Liao, Rong-Zhen
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi. Huazhong University of Science & Technology, People's Republic of China.
    Åkermark, Torbjörn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Lee, Bao-Lin
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Karlsson, Erik A.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Siegbahn, Per E. M.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Åkermark, Björn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Efficient photochemical water oxidation by a dinuclear molecular ruthenium complex2015Inngår i: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 51, nr 10, s. 1862-1865Artikkel i tidsskrift (Fagfellevurdert)
    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.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Lomoth, Reiner
    Abdel-Magied, Ahmed F.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi. Nuclear Materials Authority, Egypt.
    Rabten, Wangchuk
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Laine, Tanja M.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Chen, Hong
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK). KTH Royal Institute of Technology, Sweden.
    Sun, Junliang
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Andersson, Pher G.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Kärkäs, Markus D.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Johnston, Eric V.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Åkermark, Björn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Catalyst-solvent interactions in a dinuclear Ru-based water oxidation catalyst2016Inngår i: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 45, nr 47, s. 19024-19033Artikkel i tidsskrift (Fagfellevurdert)
    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.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Hu, Shichao
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Athanassiadis, Ioannis
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Laine, Tanja M.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Johnsson, Mats
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    An Oxofluoride Catalyst Comprised of Transition Metals and a Metalloid for Application in Water Oxidation2015Inngår i: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 21, nr 37, s. 12991-12995Artikkel i tidsskrift (Fagfellevurdert)
    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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