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  • 1.
    Abdel-Magied, Ahmed F.
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Arafa, Wael A. A.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Laine, Tanja M.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Shatskiy, Andrey
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Kärkäs, Markus D.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Åkermark, Björn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Johnston, Eric V.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Substituent Effects in Molecular Ruthenium Water Oxidation Catalysts Based on Amide Ligands2017Inngår i: ChemCatChem, ISSN 1867-3880, E-ISSN 1867-3899, Vol. 9, nr 9, s. 1583-1587Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    The production of clean and sustainable energy is considered as one of the most urgent issues for our society. Mastering the oxidation of water to dioxygen is essential for the production of solar fuels. A study of the influence of the substituents on the catalytic activity of a series of mononuclear Ru complexes (2a-e) based on a tetradentate ligand framework is presented. At neutral pH, using [Ru(bpy)(3)](PF6)(3) (bpy=2,2'-bipyridine) as the terminal oxidant, a good correlation between the turnover frequency (TOF) and the Hammett sigma(meta) parameters was obtained. Additionally, a general pathway for the deactivation of Ru-based catalysts 2a-e during the catalytic oxidation of water through poisoning by carbon monoxide was demonstrated. These results highlight the importance of ligand design for fine-tuning the catalytic activity of water oxidation catalysts.

  • 2.
    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.

  • 3. 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+).

  • 4.
    Gustafson, Karl P. J.
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Shatskiy, Andrey
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Verho, Oscar
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Kärkäs, Markus D.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Schluschass, Bastian
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Tai, Cheuk-Wai
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Åkermark, Björn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Bäckvall, Jan-Erling
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Johnston, Eric V.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Water oxidation mediated by ruthenium oxide nanoparticles supported on siliceous mesocellular foam2017Inngår i: Catalysis Science & Technology, ISSN 2044-4753, E-ISSN 2044-4761, Vol. 7, nr 1, s. 293-299Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Artificial photosynthesis is an attractive strategy for converting solar energy into fuel. In this context, development of catalysts for oxidation of water to molecular oxygen remains a critical bottleneck. Herein, we describe the preparation of a well-defined nanostructured RuO2 catalyst, which is able to carry out the oxidation of water both chemically and photochemically. The developed heterogeneous RuO2 nanocatalyst was found to be highly active, exceeding the performance of most known heterogeneous water oxidation catalysts when driven by chemical or photogenerated oxidants.

  • 5.
    Iqbal, M. Naeem
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi. Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Abdel-Magied, Ahmed F.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Abdelhamid, Hani Nasser
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Olsén, Peter
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Shatskiy, Andrey
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Zou, Xiaodong
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Åkermark, Björn
    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.
    Mesoporous Ruthenium Oxide: A Heterogeneous Catalyst for Water Oxidation2017Inngår i: ACS Sustainable Chemistry & Engineering, ISSN 2168-0485, Vol. 5, nr 11, s. 9651-9656Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Herein we report the synthesis of mesoporous ruthenium oxide (MP-RuO2) using a template-based approach. The catalytic efficiency of the prepared MP-RuO2 was compared to commercially available ruthenium oxide nanoparticles (C-RuO2) as heterogeneous catalysts for water oxidation. The results demonstrated superior performance of MP-RuO2 for oxygen evolution compared to the C-RuO2 with respect to recyclability, amount of generated oxygen, and stability over several catalytic runs.

  • 6.
    Olsén, Peter
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Morvan, Jennifer
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Sawadjoon, Supaporn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Shatskiy, Andrey
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Johnston, Eric V.
    Åkermark, Björn
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Cyclic allylic carbonates as a renewable platform for protecting chemistry in water2018Inngår i: Green Chemistry, ISSN 1463-9262, E-ISSN 1463-9270, Vol. 20, nr 14, s. 3186-3190Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    The present work explores different cyclic allylic carbonates as a potential class of allylcarbamate precursors. The 5-membered carbonate formed a carbamate with very good thermal and pH stability, which could be cleanly deprotected in aqueous solution, in just 30 min with 2 mol% Pd(OAc)(2) as catalyst. The polar nature of the installed motif made it possible to deprotect highly unpolar substrates in water as solvent.

  • 7.
    Shatskiy, Andrey
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Highly Active Ruthenium-Based Water Oxidation Catalyst with an Easy Access to the Catalytically Active SpeciesManuskript (preprint) (Annet vitenskapelig)
    Abstract [en]

    Herein is described a highly active ruthenium-based water oxidation catalyst [RuIV(mcbp)(O)(py)2] (5, mcbp2− = 2,6-bis(1-methyl-4-(carboxylate)benzimidazol-2-yl)pyridine), which can be generated from either [RuII(mcbp)(py)2] (4II) or [RuIII(Hmcbp)(py)2]2+ (4III). Complexes 4II and 4III were isolated and characterized by single crystal X-ray analysis, NMR, UV-vis, FT-IR, ESI-HRMS, EPR, and elemental analysis, and their redox properties were studied in detail by electrochemical and spectroscopic methods. Unlike for the parent catalyst [Ru(tda)(py)2] (1, tda2− = [2,2′:6′,2″-terpyridine]-6,6″-dicarboxylate), for which full transformation to the catalytically active species [RuIV(tda)(O)(py)2] (2) could not be carried out — stoichiometric generation of the catalytically active Ru-aqua complex 5 from 4II was achieved under mild conditions (pH 7.0) and short reaction times. The redox properties of the catalyst were studied and its activity for electrocatalytic water oxidation was evaluated, reaching TOFmax ≈ 40 000 s−1 at pH 9.0 (from the foot-of-the-wave analysis, FOWA), which is comparable to the activity of the state-of-the-art catalyst 2.

  • 8.
    Shatskiy, Andrey
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Ru-Based Water Oxidation Catalysts: Development and Mechanistic Studies2018Doktoravhandling, med artikler (Annet vitenskapelig)
    Abstract [en]

    Oxidation of water constitutes one of the most challenging processes in artificial photosynthesis, which aims at storing solar energy in the form of chemical bonds of high-energy fuels. To facilitate this process, efficient and durable water oxidation catalysts have to be developed and integrated into the complete photosynthetic cells. Importantly, the intricate complexity of such devices requires the catalyst not only to be highly efficient and robust, but also operate through a well-defined mechanism.

    This thesis describes the development and mechanistic studies of new water oxidation catalysts based on ruthenium. The first part of the thesis describes the synthesis of a dinuclear ruthenium-based catalyst active for both chemical and light-driven water oxidation. This catalyst displayed a pronounced influence of the acetonitrile co-solvent on the redox properties, which was studied in detail by electrochemical methods. In the second part, a new benzimidazole-based mononuclear catalyst was evaluated. The activity of the catalyst was studied for chemical and light-driven water oxidation, and insight into the operating mechanism was provided with the help of density functional theory calculations. In the third part of the thesis, a new mononuclear ruthenium-based catalyst was prepared and evaluated for electrochemically-driven water oxidation. This catalyst displayed activity similar to that of the current state-of-the-art water oxidation catalyst, while eliminating its main drawback, that is incomplete activation. The redox properties of the new catalyst were studied in detail by electrochemical and spectroscopic techniques, providing insight into the origins of its improved performance. Finally, in the fourth part of the thesis, a heterogeneous nanoparticulate catalyst immobilized on a solid support is described. The catalyst displayed high activity and stability during chemical and light-driven water oxidation, which was attributed to the small average particle size and efficient anchoring of the catalyst to the heterogeneous support via an oxidatively-stable linker.

  • 9.
    Shatskiy, Andrey
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Kivijärvi, Tove
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Lundberg, Helena
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Tinnis, Fredrik
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Adolfsson, Hans
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Ruthenium-Catalyzed Asymmetric Transfer Hydrogenation of Propargylic Ketones2015Inngår i: ChemCatChem, ISSN 1867-3880, E-ISSN 1867-3899, Vol. 7, nr 23, s. 3818-3821Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    The asymmetric transfer hydrogenation of alpha,beta-propargyl ketones catalyzed by an in situ formed ruthenium-hydroxyamide complex was explored. The acetylenic alcohols were isolated in good to excellent yields with excellent ee values (typically >90%) after short reaction times at room temperature.

  • 10.
    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.

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