2023/01/29 更新

写真a

ザキナビホアハメド ザハラン
ZakiNabeihAhmed Zahran
ZakiNabeihAhmed Zahran
所属
教育研究院 自然科学系 特任准教授
工学部 特任准教授
職名
特任准教授
外部リンク

学位

  • 博士 ( 2008年7月   オクラホマ大学 )

研究キーワード

  • Water Oxidation

  • Carbon dioxide reduction

  • Molecular complexes

  • Semiconductor photoanodes and photocathodes

  • Metal Oxides

研究分野

  • ナノテク・材料 / 無機物質、無機材料化学  / Artificial Photosynthesis

経歴

  • 新潟大学   工学部   特任准教授

    2018年4月 - 現在

 

論文

  • Distinctive Aspects in Aquation, Proton-Coupled Redox, and Photoisomerization Reactions between Geometric Isomers of Mononuclear Ruthenium Complexes with a Large-π-Conjugated Tetradentate Ligand

    Yuta Tsubonouchi, Takeumi Watanabe, Kazuha Yoshida, Shunsuke Watabe, Keisuke Inaba, Masanari Hirahara, Tsubasa Hatanaka, Yasuhiro Funahashi, Debraj Chandra, Norihisa Hoshino, Zaki N. Zahran, Masayuki Yagi

    Inorganic Chemistry   61 ( 35 )   13956 - 13967   2022年8月

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:American Chemical Society (ACS)  

    DOI: 10.1021/acs.inorgchem.2c01937

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  • Perfect Matching Factor between a Customized Double-Junction GaAs Photovoltaic Device and an Electrolyzer for Efficient Solar Water Splitting

    Zaki N. Zahran, Yugo Miseki, Eman A. Mohamed, Yuta Tsubonouchi, Kikuo Makita, Takeyoshi Sugaya, Kazuhiro Sayama, Masayuki Yagi

    ACS Applied Energy Materials   5 ( 7 )   8241 - 8253   2022年7月

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:American Chemical Society (ACS)  

    DOI: 10.1021/acsaem.2c00768

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  • Highly Efficient and Durable Electrocatalysis by a Molecular Catalyst with Long Alkoxyl Chains Immobilized on a Carbon Electrode for Water Oxidation

    Yuta Tsubonouchi, Taichi Hayasaka, Yuki Wakai, Eman. A. Mohamed, Zaki N. Zahran, Masayuki Yagi

    ACS Applied Materials & Interfaces   14 ( 13 )   15154 - 15164   2022年3月

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:American Chemical Society (ACS)  

    DOI: 10.1021/acsami.1c24263

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  • Bipyridine-based polybenzimidazole as a nitrogen-rich ionomer and a platinum nanoparticle support for enhanced fuel cell performance

    Mohamed R. Berber, Asma M. Alenad, Numa A. Althubiti, Ziyad A. Alrowaili, Zaki N. Zahran, Masayuki Yagi

    Fuel   312   122954 - 122954   2022年3月

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:Elsevier BV  

    DOI: 10.1016/j.fuel.2021.122954

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  • Nickel Sulfate as an Influential Precursor of Amorphous High-Valent Ni(III) Oxides for Efficient Water Oxidation in Preparation via a Mixed Metal-Imidazole Casting Method

    Zaki N. Zahran, Eman A. Mohamed, Tomohiro Katsuki, Yuta Tsubonouchi, Masayuki Yagi

    ACS Applied Energy Materials   5 ( 2 )   1894 - 1904   2022年1月

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:American Chemical Society (ACS)  

    DOI: 10.1021/acsaem.1c03379

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  • Characterization of electrocatalytic proton reduction and surface adsorption of platinum nanoparticles supported by a polymeric stabilizer on an ITO electrode

    Yuta Tsubonouchi, Masashi Kajita, Taichi Hayasaka, Hamada S. Mandour, Mohamed R. Berber, Zaki N. Zahran, Masayuki Yagi

    Sustainable Energy & Fuels   6 ( 3 )   815 - 821   2022年

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:Royal Society of Chemistry (RSC)  

    Pt nanoparticles stabilized by a polymeric stabilizer of polyacrylic acid were stably adsorbed on an ITO electrode to work effectively and stably for electrocatalytic proton reduction.

    DOI: 10.1039/d1se01760h

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  • A highly efficient and stable platinum film deposited <i>via</i> a mixed metal-imidazole casting method as a benchmark cathode for electrocatalytic hydrogen evolution

    Zaki N. Zahran, Eman A. Mohamed, Tomohiro Katsuki, Yuta Tsubonouchi, Debraj Chandra, Norihisa Hoshino, Masayuki Yagi

    Sustainable Energy &amp; Fuels   2022年

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:Royal Society of Chemistry (RSC)  

    A Pt cathode (Pt(w-MeIm)) prepared by a mixed metal-imidazole casting (MiMIC) method showed a remarkably superior hydrogen evolution reaction (HER) performance compared to the cathode prepared without imidazole (Pt(w/o-MeIm)), and the common Pt-based benchmark cathodes of Pt/C or the Pt plate.

    DOI: 10.1039/d2se00803c

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  • Mechanism of H+ dissociation–induced O–O bond formation via intramolecular coupling of vicinal hydroxo ligands on low-valent Ru(III) centers

    Yuki Tanahashi, Kosuke Takahashi, Yuta Tsubonouchi, Shunsuke Nozawa, Shin-ichi Adachi, Masanari Hirahara, Eman A. Mohamed, Zaki N. Zahran, Kenji Saito, Tatsuto Yui, Masayuki Yagi

    Proceedings of the National Academy of Sciences   118 ( 52 )   e2113910118 - e2113910118   2021年12月

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:Proceedings of the National Academy of Sciences  

    The understanding of O–O bond formation is of great importance for revealing the mechanism of water oxidation in photosynthesis and for developing efficient catalysts for water oxidation in artificial photosynthesis. The chemical oxidation of the Ru<sup>II</sup><sub>2</sub>(OH)(OH<sub>2</sub>) core with the vicinal OH and OH<sub>2</sub> ligands was spectroscopically and theoretically investigated to provide a mechanistic insight into the O–O bond formation in the core. We demonstrate O–O bond formation at the low-valent Ru<sup>III</sup><sub>2</sub>(OH) core with the vicinal OH ligands to form the Ru<sup>II</sup><sub>2</sub>(μ-OOH) core with a μ-OOH bridge. The O–O bond formation is induced by deprotonation of one of the OH ligands of Ru<sup>III</sup><sub>2</sub>(OH)<sub>2</sub> via intramolecular coupling of the OH and deprotonated O<sup>−</sup> ligands, conjugated with two-electron transfer from two Ru<sup>III</sup> centers to their ligands. The intersystem crossing between singlet and triple states of Ru<sup>II</sup><sub>2</sub>(μ-OOH) is easily switched by exchange of H<sup>+</sup> between the μ-OOH bridge and the auxiliary backbone ligand.

    DOI: 10.1073/pnas.2113910118

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  • Mechanisms of Photoisomerization and Water Oxidation Catalysis of Ruthenium(II) Aquo Complexes

    Yuta Tsubonouchi, Eman A. Mohamed, Zaki N. Zahran, Masayuki Yagi

    Ruthenium - an Element Loved by Researchers [Working Title]   2021年9月

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    掲載種別:論文集(書籍)内論文   出版者・発行元:IntechOpen  

    Polypyridyl ruthenium(II) complexes have been widely researched as promising functional molecules. We have found unique photoisomerization reactions of polypyridyl ruthenium(II) aquo complexes. Recently we have attempted to provide insight into the mechanism of the photoisomerization of the complexes and distinguish between the distal−/proximal-isomers in their physicochemical properties and functions. Moreover, polypyridyl ruthenium(II) aquo complexes have been intensively studied as active water oxidation catalysts (WOCs) which are indispensable for artificial photosynthesis. The catalytic aspect and mechanism of water oxidation by the distal-/proximal-isomers of polypyridyl ruthenium(II) aquo complexes have been investigated to provide the guided thought to develop more efficient molecular catalysts for water oxidation. The recent progress on the photoisomerization and water oxidation of polypyridyl ruthenium(II) aquo complexes in our group are reviewed to understand the properties and functions of ruthenium complexes.

    DOI: 10.5772/intechopen.99730

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  • Facile Fabrication of a Highly Crystalline and Well-Interconnected Hematite Nanoparticle Photoanode for Efficient Visible-Light-Driven Water Oxidation

    Tomohiro Katsuki, Zaki N. Zahran, Kou Tanaka, Tatsuya Eo, Eman A. Mohamed, Yuta Tsubonouchi, Mohamed R. Berber, Masayuki Yagi

    ACS Applied Materials & Interfaces   13 ( 33 )   39282 - 39290   2021年8月

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:American Chemical Society (ACS)  

    DOI: 10.1021/acsami.1c08949

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  • Highly selective electrocatalysis for carbon dioxide reduction to formic acid by a Co(II) complex with an equatorial N4 ligand

    Yuta Tsubonouchi, Daiki Takahashi, Mohamed R. Berber, Eman A. Mohamed, Zaki N. Zahran, Asma M. Alenad, Numa A. Althubiti, Masayuki Yagi

    Electrochimica Acta   138545 - 138545   2021年5月

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:Elsevier BV  

    DOI: 10.1016/j.electacta.2021.138545

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  • Handy Protocol of Nitrogen-Doped BiVO4 Photoanode for Visible Light-Driven Water Oxidation

    Tatsuya Eo, Tomohiro Katsuki, Mohamed R. Berber, Zaki N. Zahran, Eman A. Mohamed, Yuta Tsubonouchi, Asma M. Alenad, Numa A. Althubiti, Masayuki Yagi

    ACS Applied Energy Materials   4 ( 4 )   2983 - 2989   2021年4月

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:American Chemical Society (ACS)  

    DOI: 10.1021/acsaem.1c00261

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  • Concisely Synthesized FeNiWOx Film as a Highly Efficient and Robust Catalyst for Electrochemical Water Oxidation

    Zaki N. Zahran, Eman A. Mohamed, Yuta Tsubonouchi, Manabu Ishizaki, Takanari Togashi, Masato Kurihara, Kenji Saito, Tatsuto Yui, Masayuki Yagi

    ACS Applied Energy Materials   4 ( 2 )   1410 - 1420   2021年2月

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:American Chemical Society (ACS)  

    DOI: 10.1021/acsaem.0c02628

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  • Electrocatalytic water splitting with unprecedentedly low overpotentials by nickel sulfide nanowires stuffed into carbon nitride scabbards

    Zaki Zahran, Eman Mohamed, Yuta Tsubonouchi, Manabu Ishizaki, Takanari Togashi, Masato Kurihara, Kenji Saito, Tatsuto Yui, Masayuki Yagi

    Energy & Environmental Science   14 ( 10 )   5358 - 5365   2021年

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:Royal Society of Chemistry (RSC)  

    <p>Electrocatalytic water splitting to oxygen and hydrogen has much attention as one of the most promising approaches for sustainable production of hydrogen as a carbon-neutral fuel. To establish efficient electrocatalytic...</p>

    DOI: 10.1039/d1ee00509j

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  • A flexible cofacial Fe porphyrin dimer as an extremely efficient and selective electrocatalyst for the CO2 to CO conversion in non-aqueous and aqueous media

    Eman A. Mohamed, Zaki N. Zahran, Yoshinori Naruta

    Journal of Materials Chemistry A   9 ( 34 )   18213 - 18221   2021年

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:Royal Society of Chemistry (RSC)  

    A cofacial iron porphyrin dimer with a flexible structure (<italic>f</italic>-Fe<sub>2</sub>PD) showed extremely efficient CO<sub>2</sub>-to-CO conversion in aqueous and nonaqueous media compared to the one with a rigid structure (<italic>r</italic>-Fe<sub>2</sub>PD) and reported catalysts.

    DOI: 10.1039/d1ta04176b

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  • High Potential-Applied Catalyst Behavior of a Mononuclear Ruthenium(II) Complex on a Mesoporous ITO Electrode for Water Oxidation

    Yuta Tsubonouchi, Yuki Tanahashi, Tatsuya Eo, Junichiro Honta, Taisei Sato, Eman A. Mohamed, Zaki N. Zahran, Kenji Saito, Tatsuto Yui, Masayuki Yagi

    Journal of The Electrochemical Society   167 ( 16 )   166515 - 166515   2020年12月

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:The Electrochemical Society  

    DOI: 10.1149/1945-7111/abd3ba

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    その他リンク: https://iopscience.iop.org/article/10.1149/1945-7111/abd3ba/pdf

  • Efficient Electrocatalytic Water Oxidation by a Dinuclear Ruthenium(II) Complex with Vicinal Aquo and Hydroxo Groups Adsorbed on a TiO2 Electrode

    Yuki Tanahashi, Sho Nagai, Yuta Tsubonouchi, Masanari Hirahara, Taisei Sato, Eman A. Mohamed, Zaki N. Zahran, Kenji Saito, Tatsuto Yui, Masayuki Yagi

    ACS Applied Energy Materials   3 ( 12 )   12172 - 12184   2020年12月

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    掲載種別:研究論文(学術雑誌)   出版者・発行元:American Chemical Society (ACS)  

    DOI: 10.1021/acsaem.0c02242

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  • Molecular aspects, electrochemical properties and water oxidation catalysis on a nanoporous TiO<inf>2</inf> electrode anchoring a mononuclear ruthenium(II) aquo complex 査読

    Yuta Tsubonouchi, Tatsuya Eo, Junichiro Honta, Taisei Sato, Eman A. Mohamed, Zaki N. Zahran, Kenji Saito, Tatsuto Yui, Masayuki Yagi

    Journal of Photochemistry and Photobiology A: Chemistry   400   2020年9月

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    掲載種別:研究論文(学術雑誌)  

    © 2020 A mononuclear Ru aquo complex, [Ru(C8Otpy)(H2dcbpy)(OH2)]2+ (C8Otpy = 4′-octyloxy-2,2′:6′,2′′-terpyridine, H2dcbpy = 4,4′-dicarboxy-2,2′-bipyridine) was stably adsorbed on a nanoporous TiO2 surface to afford a TiO2 electrode anchoring the complex. The adsorption isothermal of the complex on the TiO2 surface was analyzed by the Langmuir adsorption model to provide a maximum coverage of Гmax = 4.4 × 10−8 mol cm−2 and an adsorption equilibrium constant of Kads = 1.1 × 104 M−1, suggesting that the monolayer of the complex is formed on the TiO2 surface. The cyclic voltammetry measurement of the complex on the TiO2 surface suggested the diffusion-controlled charge transport via electron hopping between the complexes through the TiO2 layer. Pourbaix diagram showed that the complex undergoes a non-H+-coupled 1e- redox reaction of a RuIIOH/RuIIIOH pair of the complex on the TiO2 electrode due to pH buffering ability of the TiO2 surface in a range of pH 5−11. Bulk electrolysis at 1.7 V vs Ag/AgCl using the complex-anchoring TiO2 electrode provided a high and steady catalytic current density of 0.39 mA cm−2 with 83 % Faradaic efficiency for O2 evolution during 1 h electrolysis. However, we presume that the complex is transformed to RuOx nanoparticles on the TiO2 electrode during the electrocatalysis, on the basis of our earlier report on the complex / mesoporous ITO electrode system (Dalton Trans., 2020, 49, 1416−1423.). The RuOH/TiO2 electrode is the efficient anode for water oxidation under the acidic conditions, irrespective of the molecular catalyst of RuOH and the alternative catalysts formed via its oxidative transformation.

    DOI: 10.1016/j.jphotochem.2020.112696

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  • Highly Efficient and Selective Electrocatalytic CO2-to-CO Conversion by a Non-heme Iron Complex with an In-Plane N-4 Ligand in Heterogeneous Aqueous Media 査読

    Eman A. Mohamed, Zaki N. Zahran, Yuta Tsubonouchi, Kenji Saito, Tatsuto Yui, Masayuki Yagi

    ACS APPLIED ENERGY MATERIALS   3 ( 5 )   4114 - 4120   2020年5月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)   出版者・発行元:AMER CHEMICAL SOC  

    A non-heme Fe complex with a tetradentate dicarboxamide N-4 in-plane ligand works efficiently and selectively for the electrocatalytic CO2-to-CO conversion in a homogeneous DMF solution. The complex was immobilized on a nitrogen-doped graphene (N-G) to achieve a CO2-to-CO conversion in neutral aqueous NaHCO3 solutions, affording CO with Faradaic efficiency of 90%, a current density of 6 mA cm(-2), and a turnover frequency of 2.1 s(-1), at an overpotential of 0.47 V, which is among those of the hitherto-reported efficient and selective Fe complexes electrocatalysts.

    DOI: 10.1021/acsaem.9b02548

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  • Multi-potential-step chronocoulospectrometry for electrocatalytic water oxidation by a mononuclear ruthenium aquo complex immobilized on a mesoporous ITO electrode. 査読 国際誌

    Yuta Tsubonouchi, Junichiro Honta, Taisei Sato, Eman A Mohamed, Zaki N Zahran, Kenji Saito, Tatsuto Yui, Masayuki Yagi

    Dalton transactions (Cambridge, England : 2003)   49 ( 5 )   1416 - 1423   2020年2月

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    記述言語:英語  

    A new mononuclear Ru aquo complex [Ru(C8Otpy)(H2dcbpy)(OH2)]2+ with 4,4'-dicarboxy-2,2'-bipyridine (H2dcbpy) and 4'-octyloxy-2,2':6',2''-terpyridine (C8Otpy) ligands was synthesized to investigate electrocatalytic water oxidation by the complex immobilized on a mesoporous indium-doped tin oxide (meso-ITO) electrode using a multi-potential-step chronocoulospectrometric (MPSCCS) technique. UV-visible absorption spectroscopic data indicated that [Ru(C8Otpy)(dcbpy)(OH2)] (RuOH2) is deprotonated to [Ru(C8Otpy)(dcbpy)(OH)]- (RuOH) on the meso-ITO surface even at pH 5.9 of the electrolyte solution. The cyclic voltammogram (CV) of the RuOH/meso-ITO electrode showed a pH-independent redox response at E1/2 = 0.80 V vs. Ag/AgCl in the pH range of 5-12, being assigned to a non-proton-coupled 1e- redox process of RuIIOH/RuIIIOH. The MPSCCS measurement of the RuOH/meso-ITO electrode between 0.2 and 1.5 V vs. Ag/AgCl showed that RuIV species (tentatively RuIVO) exist in a steady state of the electrocatalysis in the initial stage. This suggests that the electrochemical oxidation from RuIVO to RuVO could compete with the water nucleophilic attack for O-O bond formation involved in the rate-determining step under the employed conditions. The possibility that the water nucleophilic attack on RuIVO could also compete with the electrochemical oxidation of RuIVO to RuVO was suggested by the electrocatalytic water oxidation at a low applied potential of 1.4 V prior to the formation potential of RuVO. The MPSCCS measurement at 1.4 V for 1 h showed that RuOH is gradually transformed into an alternative catalyst (most likely RuOx nanoparticles) on the electrode. The MPSCCS technique is promising to reveal the redox reactions and catalytic aspects of molecular catalysts immobilized on an electrode for water oxidation.

    DOI: 10.1039/c9dt04442f

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  • Critical Hammett Electron-Donating Ability of Substituent Groups for Efficient Water Oxidation Catalysis by Mononuclear Ruthenium Aquo Complexes 査読

    Watabe Shunsuke, Tanahashi Yuki, Hirahara Masanari, Yamazaki Hirosato, Takahashi Kosuke, Mohamed Eman A, Tsubonouchi Yuta, Zahran Zaki N, Saito Kenji, Yu Tatsuto, Yagi Masayuki

    INORGANIC CHEMISTRY   58 ( 19 )   12716 - 12723   2019年10月

  • Characterization and mechanism of efficient visible-light-driven water oxidation on an in situ N2-intercalated WO3 nanorod photoanode 査読

    ザハラン ザキナビハアハメド

    ACS Sustainable Chemistry & Engineering   2019年10月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    添付ファイル: acssuschemeng.9b04467.pdf

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  • Critical Hammett Electron-Donating Ability of Substituent Groups for Efficient Water Oxidation Catalysis by Mononuclear Ruthenium Aquo Complexes 査読

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    Inorganic chemistry   58 ( 19 )   12716 - 12723   2019年9月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    添付ファイル: acs.inorgchem.9b01623.pdf

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  • Recent Advances in the Development of Molecular Catalyst‐Based Anodes for Water Oxidation toward Artificial Photosynthesis 査読

    ザハラン ザキナビハアハメド

    ChemSusChem   12 ( 9 )   1775 - 1793   2019年5月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1002/cssc.201802795

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  • Efficient Solar‐Assisted O2 Reduction Using a Cofacial Iron Porphyrin Dimer Catalyst Integrated into a p‐CuBi2O4 Photocathode 査読

    ザハラン ザキナビハアハメド

    Chemistry–A European Journal   24 ( 42 )   10606 - 10611   2018年7月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1002/chem.201704143

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  • Efficient Photoelectrochemical O2 and CO Production Using BiVO4 Water Oxidation Photoanode and CO2 Reduction Au Nanoparticle Cathode Prepared by In Situ Deposition from Au3+ Containing Solution 査読

    ザハラン ザキナビハアハメド

    Advanced Sustainable Systems   1 ( 11 )   1700111   2017年11月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1002/adsu.201700111

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  • Enhanced Performance of Pristine Ta3N5 Photoanodes for Solar Water Splitting by Modification with Fe–Ni–Co Mixed-Metal Oxide Cocatalysts 査読

    ザハラン ザキナビハアハメド

    The Journal of Physical Chemistry C   121 ( 37 )   20093 - 20100   2017年9月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1021/acs.jpcc.7b04403

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  • Electrocatalytic water oxidation at low energy cost by a highly active and robust calcium-manganese oxide thin film sintered on an FTO electrode with ethyl methyl imidazolium triflate ionic liquid 査読

    Zaki N. Zahran, Eman A. Mohamed, Yoshinori Naruta

    JOURNAL OF MATERIALS CHEMISTRY A   5 ( 29 )   15167 - 15174   2017年8月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)   出版者・発行元:ROYAL SOC CHEMISTRY  

    We report a simple and novel method involving an ethyl methyl imidazolium triflate ionic liquid (EMI OTf) to prepare highly mechanically stable crystalline alpha-Mn2O3 and calcium-incorporated manganese oxide (CaMn-oxide) thin film water oxidation electrocatalysts (WOCs) on a fluorine-doped tin oxide (FTO) electrode (FTO/EMI alpha-Mn2O3 and FTO/EMI CaMn-oxide). Electrochemical measurements showed that the incorporation of calcium into manganese oxide promotes water oxidation at a very low energy cost, similar to that observed in natural photosystem II (PSII). The low energy cost is due to the involvement of the Mn-IV=O species in the catalysis as compared to the Mn-V=O species that has been previously detected in calcium-free alpha-Mn2O3. Moreover, the FTO/EMI CaMn-oxide electro-catalyst showed unprecedentedly high activity (TOF approximate to 29.8 s(-1) at eta = 0.57 V) and robustness (tested for 40 h) for water oxidation in a neutral potassium phosphate (KPi) buffer solution (0.1 M, pH 7.0). The mechanism of water oxidation by FTO/EMI CaMn-oxide was discussed and applied for water oxidation by the mu-oxido-CaMn4O5 cluster of photosystem II (PS II).

    DOI: 10.1039/c7ta03665e

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  • Covalent bonds immobilization of cofacial Mn porphyrin dimers on an ITO electrode for efficient water oxidation in aqueous solutions 査読

    Eman A. Mohamed, Zaki N. Zahran, Yoshinori Naruta

    JOURNAL OF CATALYSIS   352   293 - 299   2017年8月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)   出版者・発行元:ACADEMIC PRESS INC ELSEVIER SCIENCE  

    We previously reported several manganese porphyrin dimers as the first manganese-containing molecular catalysts for water oxidation, however, in non-aqueous CH3CN solution containing 5% H2O. Here, we successfully fabricated these dimers with mono- and hexaphosphonic acid groups, Mn2DP-PO3H2 and Mn2DP-(PO3H2)(6), to covalently assemble them on the surface of ITO electrode (ITO = indium-doped tin oxide) and use the Mn2DP-PO3H2 and Mn2DP-(PO3H2)(6)vertical bar ITO assemblies as heterogeneous catalysts for electrochemical water oxidation in aqueous buffer solutions. The mono-phosphonic acid fabricated assemblies showed unprecedent high turnover frequencies (TOFs) (up to 44.9 s(-1)) at a low overpotential (eta= 0.47 V) in a neutral buffer solution. In acidic buffered solutions (pH = 1.5), they showed higher TOFs (up to 47.4 s(-1)) at a very low overpotential (eta = 0.26 V). The robustness of the mono-phosphonic acid fabricated catalysts, Mn2DP-PO3H2 vertical bar ITO, was tested at a high overpotential (eta = 0.80 V). Although they showed an oxygen evolution with 178.3 s(-1) TOF, the oxygen evolution completely stopped after 11 h electrolysis. UV-vis spectra monitored during the electrolysis clearly indicated the gradual detachment of the catalysts from the ITO surface is likely the main reason of stopping the oxygen evolution. The hexa-phosphonic acid catalyst assembly, Mn2DP-(PO3N2)(6)vertical bar ITO, however, showed a continuous oxygen evolution without stopping even after 23 h of electrolysis with 199.3 s(-1) TOF. Tafel plots in different pHs give insights on the mechanism of H2O oxidation. (C) 2017 Elsevier Inc. All rights reserved.

    DOI: 10.1016/j.jcat.2017.05.018

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  • Efficient Heterogeneous CO2 to CO Conversion with a Phosphonic Acid Fabricated Cofacial Iron Porphyrin Dimer 査読

    ザハラン ザキナビハアハメド

    Chemistry of Materials   29 ( 17 )   7140 - 7150   2017年8月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

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  • Simple preparation of highly active water splitting FTO/BiVO4 photoanode modified with tri-layer water oxidation catalysts 査読

    Eman A. Mohamed, Zaki N. Zahran, Yoshinori Naruta

    JOURNAL OF MATERIALS CHEMISTRY A   5 ( 15 )   6825 - 6831   2017年4月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)   出版者・発行元:ROYAL SOC CHEMISTRY  

    A colloidal BiVO4 solution, prepared from equimolar mixing of Bi(NO3)(3)center dot 5H(2)O and NH4VO3 in MeOH containing 15% (v/v) 1-ethyl-3-methylimidazolium trifluoromethanesulfonate (EMI triflate) ionic liquid, was coated on a fluorine-doped tin oxide conducting glass (FTO) with a doctor blade technique; itwas sintered at 450 degrees C for 2 h to produce a super highly mechanically stable film of nanocrystalline scheelite-monoclinic, s-m BiVO4 photoanode. This technique endowed an excellent solar-driven water splitting activity for both the bare photoanode and that modified with tri-layers of non-precious water oxidation catalysts. The presence of EMI triflate in the precursor solution is essential for the mechanical stability of the film. Moreover, carbon, nitrogen, and oxygen of the EMI triflate were left over in the resulting film, and they did not affect its crystalline phase.

    DOI: 10.1039/c7ta00156h

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  • Kinetics and Mechanism of Heterogeneous Water Oxidation by alpha-Mn2O3 Sintered on an FTO Electrode 査読

    Zaki N. Zahran, Eman A. Mohamed, Yoshinori Naruta

    ACS CATALYSIS   6 ( 7 )   4470 - 4476   2016年7月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)   出版者・発行元:AMER CHEMICAL SOC  

    Kinetic studies of heterogeneous water oxidation by an alpha-Mn2O3/FTO electrocatalyst in nonaqueous (CH3CN/0.1 M n-Bu4NPF6 and DMF/0.1 M n-Bu4NPF6) and aqueous 0.1 M KPi (pH 7.0) solutions showed that the rate of water oxidation is first order in catalyst concentration and in H2O concentration. The square wave and cyclic voltammetry measurements reveal the stepwise proton-coupled electron transfer (PCET) oxidations of the active Mn-II-OH2 site to Mn-III-OH and then to Mn-IV=O and finally an electron transfer oxidation of Mn-IV=O to Mn-V=O species. The Mn-V=O species undergoes a rate-limiting O atom transfer to H2O to give a Mn-III-OOH2 species that, in turn, undergoes further oxidations to release O-2.

    DOI: 10.1021/acscatal.6b00413

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  • Kinetics and Mechanism of Heterogeneous Water Oxidation by α-Mn2O3 Sintered on an FTO Electrode 査読

    ザハラン ザキナビハアハメド

    ACS Catalysis   6 ( 7 )   4470 - 4476   2016年6月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

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  • Bio-inspired cofacial Fe porphyrin dimers for efficient electrocatalytic CO2 to CO conversion: Overpotential tuning by substituents at the porphyrin rings 査読

    Zaki N. Zahran, Eman A. Mohamed, Yoshinori Naruta

    SCIENTIFIC REPORTS   6   24533   2016年4月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)   出版者・発行元:NATURE PUBLISHING GROUP  

    Efficient reduction of CO2 into useful carbon resources particularly CO is an essential reaction for developing alternate sources of fuels and for reducing the greenhouse effect of CO2. The binuclear Ni, Fe-containing carbon monoxide dehydrogenase (CODHs) efficiently catalyzes the reduction of CO2 to CO. The location of Ni and Fe at proper positions allows their cooperation for CO2 to CO conversion through a push-pull mechanism. Bio-inspired from CODHs, we used several cofacial porphyrin dimers with different substituents as suitable ligands for holding two Fe ions with suitable Fe-Fe separation distance to efficiently and selectively promote CO2 to CO conversion with high turnover frequencies, TOFs. The substituents on the porphyrin rings greatly affect the catalysis process. By introducing electron-withdrawing/-donating groups, e.g. electron-withdrawing perfluorophenyl, at all meso positions of the porphyrin rings, the catalysis overpotential,. was minimized by approximate to 0.3 V compared to that obtained by introducing electron-donating mesityl groups. The Fe porphyrin dimers among reported catalysts are the most efficient ones for CO2 to CO conversion. Control experiments indicate that the high performance of the current CO2 to CO conversion catalysts is due to the presence of binuclear Fe centers at suitable Fe-Fe separation distance.

    DOI: 10.1038/srep24533

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  • Electrocatalytic Water Oxidation by a Highly Active and Robust -Mn2O3 Thin Film Sintered on a Fluorine-Doped Tin Oxide Electrode 査読

    Zaki N. Zahran, Eman A. Mohamed, Takehiro Ohta, Yoshinori Naruta

    CHEMCATCHEM   8 ( 3 )   532 - 535   2016年2月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)   出版者・発行元:WILEY-V C H VERLAG GMBH  

    As a water oxidation catalyst, -Mn2O3 has higher activity than other manganese oxides. However, the robustness of the catalyst supported on conducting electrodes has only been tested for a short time (1h) and it shows a gradual decrease in activity. Furthermore, the turnover number (TON) and turnover frequency (TOF) have not been reported. Herein, we optimized the preparation of transparent nanocrystalline -Mn2O3 on a fluorine-doped tin oxide (FTO) electrode, and this resulting catalyst shows, in neutral aqueous 0.1m potassium phosphate buffer solution, a high electrocatalytic water oxidation activity with a TON of 230, a TOF of 5.3x10(-3)s(-1) based on the all-Mn content, and a TOF of 2.1s(-1) based on the amount of surface-active Mn with a Faradic efficiency of 96.7% at an overpotential of 470mV. The robustness of the -Mn2O3/FTO electrocatalyst was tested for a long time (80h) without a decrease in activity.

    DOI: 10.1002/cctc.201501073

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  • Electrocatalytic water oxidation at low energy cost by a highly active and robust calcium–manganese oxide thin film sintered on an FTO electrode with ethyl methyl imidazolium triflate ionic liquid 査読

    ザハラン ザキナビハアハメド

    ChemCatChem   8 ( 3 )   532 - 535   2016年2月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

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  • Efficient electrocatalytic CO2 reduction with a molecular cofacial iron porphyrin dimer 査読

    Eman A. Mohamed, Zaki N. Zahran, Yoshinori Naruta

    CHEMICAL COMMUNICATIONS   51 ( 95 )   16900 - 16903   2015年

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    記述言語:英語   掲載種別:研究論文(学術雑誌)   出版者・発行元:ROYAL SOC CHEMISTRY  

    A cofacial iron tetraphenyl porphyrin dimer, o-Fe2DTPP, bio-inspired by the Ni-Fe containing metalloenzyme, carbon monoxide dehydrogenase (CODH), efficiently and selectively catalyses the electrochemical reduction of CO2 to CO in DMF/10% H2O solution at the electro-generated Fe-0(por) species with high Faradic efficiency (95%) and TOF (4300 s(-1)) at a moderate overpotential, eta = 0.66 V.

    DOI: 10.1039/c5cc04273a

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  • Effects of temperature of heat treatment on surface nano-structure of Ti metal electrode formed by alkali, acid and heat treatments 査読

    ザハラン ザキナビハアハメド

    ICEAS 1331   841 - 844   2012年

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    記述言語:英語   掲載種別:研究論文(国際会議プロシーディングス)  

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  • Bis (1-methyl-1H-imidazole-κN3)[N, N′-o-phenylenebis (pyridine-2-carboxamido)-κ4N] manganese (II) 査読

    ザハラン ザキナビハアハメド

    Acta Crystallographica Section E   65 ( 1 )   M75 - U807   2009年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1107/S1600536808041640

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  • Crystal structures of manganese- and cobalt-substituted myoglobin in complex with NO and nitrite reveal unusual ligand conformations 査読

    Zaki N. Zahran, Lilian Chooback, Daniel M. Copeland, Ann H. West, George B. Richter-Addo

    JOURNAL OF INORGANIC BIOCHEMISTRY   102 ( 2 )   216 - 233   2008年2月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)   出版者・発行元:ELSEVIER SCIENCE INC  

    Nitrite is now recognized as a storage pool of bioactive nitric oxide (NO). Hemoglobin (Hb) and myoglobin (Mb) convert, under certain conditions, nitrite to NO. This newly discovered nitrite reductase activity of Hb and Mb provides an attractive alternative to mammalian NO synthesis from the NO synthase pathway that requires dioxygen. We recently reported the X-ray crystal structure of the nitrite adduct of ferric horse heart Mb, and showed that the nitrite ligand binds in an unprecedented O-binding (nitrito) mode to the d(5) ferric center in Mb(III)(ONO) [D.M. Copeland, A. Soares, A.H. West, G.B. Richter-Addo, J. Inorg. Biochem. 100 (2006) 1413-1425]. We also showed that the distal pocket in Mb allows for different conformations of the NO ligand (120 degrees and 144 degrees) in Mb(II)NO depending on the mode of preparation of the compound. In this article, we report the crystal structures of the nitrite and NO adducts of man ganese-substituted hh Mb (a d(4) system) and of the nitrite adduct of cobalt-substituted hh Mb (a d(6) System). We show that the distal His64 residue directs the nitrite ligand towards the rare nitrito O-binding mode in Mn(III)Mb and Co(III)Mb. We also report that the distal pocket residues allow a stabilization of an unprecendented bent MnNO moiety in Mn(II)MbNO. These crystal structural data, when combined with the data for the aquo, methanol, and azide MnMb derivatives, provide information on the role of distal pocket residues in the observed binding modes of nitrite and NO ligands to wild-type and metal-substituted Mb. (c) 2007 Elsevier Inc. All rights reserved.

    DOI: 10.1016/j.jinorgbio.2007.08.002

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  • A bioinorganic approach to the study of the interactions of nitrogen oxides with manganese porphyrins and manganese-and cobalt-reconstituted myoglobin. 査読

    ザハラン ザキナビハアハメド

    2007年

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    記述言語:英語   掲載種別:学位論文(博士)  

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  • Specific detection of gaseous NO and (NO)-N-15 in the headspace from liquid-phase reactions involving NO-generating organic, inorganic, and biochemical samples using a mid-infrared laser 査読

    Jun Yi, Khosrow Namjou, Zaki N. Zahran, Patrick J. McCann, George B. Richter-Addo

    NITRIC OXIDE-BIOLOGY AND CHEMISTRY   15 ( 2 )   154 - 162   2006年9月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)   出版者・発行元:ACADEMIC PRESS INC ELSEVIER SCIENCE  

    Nitric oxide (NO) is an important biological signaling agent. The specific detection of NO represents a continuing challenge in the field of NO research. Many methods are currently employed for the detection of NO. Here, we report a qualitative but specific detection method for gaseous NO liberated in and from solution taking advantage of its low solubility. Importantly, our mid-infrared laser absorption method does not depend on any chemical derivatization of NO, and is applicable over a wide range of concentrations for both protein work and in organic-in organic modeling work. We also apply this method to the specific detection of (NO)-N-15. (c) 2006 Elsevier Inc. All rights reserved.

    DOI: 10.1016/j.niox.2006.01.009

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  • Synthesis, molecular structure, and redox behavior of an oxo-bridged dimer of a ruthenium-bpb nitrosyl 査読

    ZN Zahran, DR Powell, GB Richter-Addo

    INORGANICA CHIMICA ACTA   359 ( 9 )   3084 - 3088   2006年6月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)   出版者・発行元:ELSEVIER SCIENCE SA  

    We have prepared the oxo-bridged dirner [Ru(bpb)(NO](2)(mu-O) in 60% isolated yield from the reaction of the known Ru(bpb)(NO)Cl with silver nitrite. The compound exhibits a upsilon(NO) of 1758 cm(-1) (KBr pellet). The crystal structure reveals a linear ON-Ru-O-Ru-NO fragment with the oxo atom serving as an inversion center in the molecule. The redox behavior in DMF is characterized by a reversible reduction followed by a second but irreversible reduction in this solvent. (c) 2006 Elsevier B.V. All rights reserved.

    DOI: 10.1016/j.ica.2006.02.013

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  • Fiber-optic infrared spectroelectrochemical studies of six-coordinate manganese nitrosyl Porphyrins in nonaqueous media 査読

    ZN Zahran, MJ Shaw, MA Khan, GB Richter-Addo

    INORGANIC CHEMISTRY   45 ( 6 )   2661 - 2668   2006年3月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)   出版者・発行元:AMER CHEMICAL SOC  

    The redox behavior of the six-coordinate (por)Mn(NO)(1-Melm) (por = tetraphenylporphyrin dianion (TPP), tetratolylporphyrin dianion (TTP), or tetra-p-methoxyphenylporphyrin dianion (T(p-OMe)PP)) complexes were examined by cyclic voltammetry at room temperature and at -78 degrees C in two nonaqueous solvents (CH2Cl2 and THF) at a Pt disk electrode. In CH2Cl2 at room temperature, the compounds undergo four oxidations and two reductions within the solvent limit; in THF, the compounds undergo one oxidation and three reductions. In both solvents, the first oxidation represents a chemically irreversible one-electron process involving the rapid loss of nitric oxide. The oxidation occurs at the MnNO site as judged from bulk electrolysis, UV-vis spectroscopy at room temperature, and IR spectroelectrochemistry at room temperature and at -78 degrees C. The second oxidation, accessible in CH2Cl2, is also chemically irreversible and occurs at the porphyrin ring; the third and the fourth oxidations are, on the other hand, chemically reversible but also occur at the porphyrin ring. The first reduction is chemically irreversible in CH2Cl2, occurs at the porphyrin ring, and is followed by loss of NO. In THF, the first reduction is chemically reversible and is followed by reversible loss of NO.

    DOI: 10.1021/ic051190n

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  • Synthesis, characterization and molecular structures of six-coordinate manganese nitrosyl porphyrins 査読

    ZN Zahran, J Lee, SS Alguindigue, MA Khan, GB Richter-Addo

    DALTON TRANSACTIONS   ( 1 )   44 - 50   2004年

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    記述言語:英語   掲載種別:研究論文(学術雑誌)   出版者・発行元:ROYAL SOC CHEMISTRY  

    Manganese(II) porphyrins are isoelectronic with iron(II) porphyrins, and previously reported work suggests that manganese nitrosyl porphyrins are good structural models for their kinetically unstable and biologically relevant ferric - NO analogues. We have prepared a new set of six-coordinate manganese nitrosyl porphyrins of the general form (por) Mn(NO)(L) (por = TTP, T(p-OCH3) PP; L = piperidine, methanol, 1-methylimidazole) in moderate to high yields. The (por) Mn(NO)(pip) complexes were prepared from the reductive nitrosylation of the (por) MnCl compounds with NO in the presence of piperidine. The IR spectra of the (por) Mn(NO)(pip) compounds as KBr pellets show new strong bands at 1746 cm(-1) (for TTP) and 1748 cm(-1) (for (T(p-OCH3)PP) due to the NO ligands. Attempted crystallization of one of these compounds ( por = TTP) from dichloromethane - methanol resulted in the generation of the methanol complex (TTP) Mn(NO)(CH3OH). Reaction of the (por)Mn(NO)(pip) compounds with excess 1-methylimidazole gave the (por)Mn(NO)(1-MeIm) derivatives in good yields. The IR spectra of these compounds show nu(NO) bands that are similar to12 cm(-1) lower than those of the (por) Mn(NO)(pip) precursors, indicative of greater Mn --&gt; NO pi-backdonation in the 1-MeIm derivatives. X-Ray crystal structures of three of these compounds, namely (TTP) Mn(NO)(CH3OH), (TTP) Mn(NO)(1-MeIm) and (T(p-OCH3) PP) Mn(NO)(1-MeIm) were obtained, and reveal that the NO ligands in these complexes are linear.

    DOI: 10.1039/b308143p

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▶ 全件表示

書籍等出版物

  • Mechanisms of Photoisomerization and Water Oxidation Catalysis of Ruthenium(II) Aquo Complexes

    Yuta Tsubonouchi, Eman A. Mohamed, Zaki N. Zahran, Masayuki Yagi( 担当: 共著)

    2021年9月 

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  • Photoisomerization of polypyridyl ruthenium (II): aquo complexes

    ザハラン ザキナビハアハメド( 担当: 分担執筆)

    2019年 

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  • Water oxidation using molecular photocatalysts

    ザハラン ザキナビハアハメド( 担当: 分担執筆)

    2019年 

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MISC

  • Nitrite binding to heme iron: Structural insights

    Geome Richter-Addo, Jun Eva Yi, Zaki N. Zahran, Daniel M. Copeland

    NITRIC OXIDE-BIOLOGY AND CHEMISTRY   19   S28 - S28   2008年

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    記述言語:英語   掲載種別:研究発表ペーパー・要旨(国際会議)   出版者・発行元:ACADEMIC PRESS INC ELSEVIER SCIENCE  

    DOI: 10.1016/j.niox.2008.06.038

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  • Specific detection of gaseous NO and 15-NO from chemical reactions using a mid-infrared laser

    J Yi, GB Richter-Addo, K Narajou, ZN Zahran, PJ McCann

    NITRIC OXIDE-BIOLOGY AND CHEMISTRY   14 ( 4 )   A22 - A22   2006年6月

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    記述言語:英語   掲載種別:研究発表ペーパー・要旨(国際会議)   出版者・発行元:ACADEMIC PRESS INC ELSEVIER SCIENCE  

    DOI: 10.1016/j,niox.2006.04.076

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産業財産権

  • Catalysts and their preparation methods

    ザハラン ザキナビハアハメド

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    出願番号:特願2019-90888  出願日:2019年5月

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  • Preparation methods of catalysts, preparation methods of metal oxides and their catalysts

    ザハラン ザキナビハアハメド

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    出願番号:特願2019-95465  出願日:2019年5月

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受賞

  • JSPS scholarship for foreigner researcher

    2010年  

    ザハラン ザキナビハアハメド

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  • The graduate college poster award

    2003年   University of Oklahoma  

    ザハラン ザキナビハアハメド

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  • Ph.D scholarship

    The Egyptian Government Scholarship in Chemistry  

    ザハラン ザキナビハアハメド

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共同研究・競争的資金等の研究

  • Understanding and development of highly efficient water splitting catalysts with core-shell structures for solar-hydrogen production

    研究課題/領域番号:20K05684  2020年4月 - 2023年3月

    日本学術振興会  科学研究費助成事業 基盤研究(C)  基盤研究(C)

    ZAHRAN ZAKI・NABEIH・AHMED

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    配分額:4290000円 ( 直接経費:3300000円 、 間接経費:990000円 )

    The critical bottleneck for sustainable production of hydrogen has remained in sluggish oxygen evolving reaction (OER), requiring insufficiently low overpotentials, η. We succeeded in reporting a facile and versatile method for the preparation of loading-controllable metal oxide films adhered rigidly on electrode substrates, enabling effectual material hunting for superior OER anodes. This allows us to discover a ternary FeNiWOx film on a nickel foam (NF), attaining one of the lowest overpotentials of η10 = 167 (The superscripts represent the attained current densities of 10 mA cm-2) with a Tafel slope of 49 mV dec-1 and at least 100 h stability in OER, which compare advantageously with only a few state-of-the-art OER anodes with excellent η10 < 200 mV. The electrochemical data indicate synergistic coupling among ternary metal centers of Ni, Fe and W to decrease the η value. The OER current is pH-dependent for the FeNiWOx film, showing the non-proton-concerted process in the rate-determining step for OER.

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  • Developing efficient inexpensive catalysts for solar driven carbon dioxide-to-fuels conversion towards artificial photosynthesis

    研究課題/領域番号:19K21135  2019年4月 - 2020年3月

    日本学術振興会  科学研究費助成事業 研究活動スタート支援  研究活動スタート支援

    ZAHRAN ZAKI・NABEIH・AHMED

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    配分額:2990000円 ( 直接経費:2300000円 、 間接経費:690000円 )

    Here we developed several cheap iron non-porphyrin complexes, an Fe(bpb) that showed high activity for CO2 reduction with 93% CO faradaic efficiency at a moderate overpotential η = 0.41 V in homogeneous and heterogeneous media.

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  • Developing efficient inexpensive catalysts for solar driven carbon dioxide-to-fuels conversion towards artificial photosynthesis

    2018年4月 - 2020年3月

    JSPS Japan Society for the Promotion of Science 

    ザハラン ザキナビハアハメド

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    担当区分:研究代表者  資金種別:競争的資金

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