Article
Chemistry, Multidisciplinary
Jian Liu, Melissa M. Bollmeyer, Yujeong Kim, Dengmengfei Xiao, Samantha N. MacMillan, Qi Chen, Xuebing Leng, Sun Hee Kim, Lili Zhao, Kyle M. Lancaster, Liang Deng
Summary: Mononuclear Pd(I) species are potential intermediates in Pd-catalyzed reactions, and a Pd(I) amido complex has been isolated and characterized in this study, revealing its electronic features and reactivity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
McKenna K. Goetz, Joseph E. Schneider, Alexander S. Filatov, Kate A. Jesse, John S. Anderson
Summary: This study reports the isolation and characterization of a new terminal Co-III-oxo complex capable of hydroxylation of aliphatic C-H bonds. The experimental and DFT analysis reveal that the reaction is endergonic at the initial C-H activation step but driven by an extremely exergonic radical rebound step, similar to cytochrome P450 enzymes. The rapid C-H hydroxylation reactivity displayed in this well-defined system provides insight into biological systems and synthetic oxidants.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Inorganic & Nuclear
Jinjing Pan, Li Zhang, Yuhao He, Qian Yu, Gengwen Tan
Summary: Magnesium(I) complexes are widely studied as reducing agents in small-molecule activation and organometallic synthesis. Despite successfully isolating a magnesium(I) species in this study, no stable mononuclear magnesium(I) compounds have been identified, with the complex identified as essentially a magnesium(II)-radical dianion complex based on spectroscopic studies and theoretical calculations.
Article
Chemistry, Physical
Li-Li Wang, Bei Wan, Shu-Hui Lai, Lin-Fang Weng, Hai-Yang Liu, Hui Wang
Summary: This study investigates ultrafast intramolecular electron transfer in manganese(V)-oxo corrole complexes, revealing the influence of different ligands on the electron transfer rate.
Article
Chemistry, Inorganic & Nuclear
Corey A. Richards, Nigam P. Rath, Jamie M. Neely
Summary: Transition metal imide-mediated C-N bond formation is a powerful strategy for introducing nitrogen into organic compounds. Stoichiometric experiments revealed a catalyst deactivation pathway, which was suppressed in the presence of a coordinating additive. These insights were instrumental in identifying reaction conditions that allow for turnover of the iron catalyst.
Article
Chemistry, Physical
Young Hyun Hong, Yuri Jang, Roman Ezhov, Mi Sook Seo, Yong-Min Lee, Bhawana Pandey, Seungwoo Hong, Yulia Pushkar, Shunichi Fukuzumi, Wonwoo Nam
Summary: The synthesis, characterization, and electron-transfer oxidation reactivity of a chromium(V)-oxo TAML cation radical complex binding Sc3+ ion were reported. The complex demonstrated highly reactive oxidizing capability with an extremely small reorganization energy, making it one of the most powerful high-valent metal-oxo oxidants in ET and OAT reactions.
Article
Chemistry, Inorganic & Nuclear
Hua-Jie Jiang, Hendrik D. A. Simon, Elisabeth Irran, Hendrik F. T. Klare, Martin Oestreich
Summary: Based on experimental data, a refined mechanistic picture of carbonyl hydrosilylation catalyzed by a cationic rhenium(V) oxo complex introduced by Abu-Omar is presented. The role of acetonitrile ligand in the reaction and the key intermediates involved were identified.
Article
Chemistry, Inorganic & Nuclear
Wenjuan Zhu, Namita Sharma, Yong-Min Lee, Mohamed E. El-Khouly, Shunichi Fukuzumi, Wonwoo Nam
Summary: This study reports a new method for generating a nonheme iron(IV)-oxo complex using singlet oxygen instead of triplet oxygen and a hydrogen atom donor with relatively strong C-H bonds.
INORGANIC CHEMISTRY
(2023)
Article
Biochemistry & Molecular Biology
Bao-Long Chen, Sheng-Yi Yan, Xiao-Qing Zhu
Summary: This study synthesized a polypyridine mono-oxygen complex [(RuO)-O-IV](2+) and investigated the hydrogen element transfer process between the complex and organic hydride donors. Through H-1-NMR analysis and thermodynamics- and kinetics-based assessments, a thermodynamic platform was established, confirming a one-step hydride transfer reaction between [(RuO)-O-IV](2+) and the organic hydride donors. The advantages and nature of this new mechanism approach were revealed.
Article
Chemistry, Multidisciplinary
Sangmin Kim, Junho Kim, Hongyu Zhong, Grace B. Panetti, Paul J. Chirik
Summary: The synthesis of a piano-stool ruthenium hydride with dual catalytic functions is described. The addition of a neutral supporting ligand successfully prevents a deleterious reaction pathway. The ruthenium hydride is an effective catalyst for various reactions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Michal S. Dutkiewicz, Conrad A. P. Goodwin, Mauro Perfetti, Andrew J. Gaunt, Jean-Christophe Griveau, Eric Colineau, Attila Kovacs, Ashley J. Wooles, Roberto Caciuffo, Olaf Walter, Stephen T. Liddle
Summary: Neptunium, the first artificially synthesized actinide, has been less studied compared to its famous neighbors uranium and plutonium. This study reports the synthesis, isolation, and characterization of a stable molecular neptunium(V)-mono(oxo) triamidoamine complex, demonstrating the possibility of stabilizing and studying high-oxidation-state transuranic complexes with a single metal-ligand bond.
Article
Chemistry, Physical
Rinny Kuilya, Young Hyun Hong, Namita Sharma, Yong-Min Lee, Wonwoo Nam, Shunichi Fukuzumi
Summary: This study reports the formation of a long-lived photoexcited state of a MnIV-oxo complex binding triflic acid, composed of only earth-abundant elements, which exhibits the highest oxidizing reactivity among the high-valent metal-oxo species reported so far. The photoexcited state is capable of oxidizing toluene to benzyl alcohol and benzaldehyde with a quantum efficiency of 200%, making it the most efficient photooxidation reaction reported to date.
Rating: 7/10
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Guangjian Liao, Fuming Mei, Zhuqi Chen, Guochuan Yin
Summary: This study demonstrates an improved dioxygen activation by introducing Lewis acid into Fe-II(BPMEN)(OTf)(2) complex, leading to successful catalytic reactions of tryptophan 2,3-dioxygenase and olefinic CC ? bond oxygenation. The results reveal the enhanced electrophilic oxygenation capability of the putative iron(III) superoxo species through electrostatic interaction with Lewis acid.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Multidisciplinary
Hideki Ohtsu, Mikio Takaoka, Yosuke Tezuka, Kiyoshi Tsuge, Koji Tanaka
Summary: The study discovered an NAD(+)-type metal complex with oxidizing ability to convert alcohols to aldehydes and ketones, and successfully synthesized a novel zinc(II) complex with a C-C coupling ligand. Kinetic analysis based on absorption spectroscopic measurements revealed that the reaction proceeds through electron transfer followed by proton transfer mechanism.
CHEMICAL COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Joseph E. Schneider, McKenna K. Goetz, John S. Anderson
Summary: Transition metal oxo species play a crucial role in activating strong C-H bonds. While various parameters have been proposed to determine their reactivity, only thermodynamic parameters are statistically significant in influencing their ability to mediate C-H activation. Notably, the oxidation potential and basicity of the oxo complexes also make independent and significant contributions, suggesting a more complex thermodynamic landscape than previously thought.
Article
Chemistry, Inorganic & Nuclear
Dachao Hong, Yuji Ohgomori, Yoshihiro Shimoyama, Hiroaki Kotani, Tomoya Ishizuka, Yoshihiro Kon, Takahiko Kojima
INORGANIC CHEMISTRY
(2019)
Article
Chemistry, Inorganic & Nuclear
Tomoya Ishizuka, Taichi Kogawa, Misaki Makino, Yoshihito Shiota, Kazuaki Ohara, Hiroaki Kotani, Shunsuke Nozawa, Shin-ichi Adachi, Kentaro Yamaguchi, Kazunari Yoshizawa, Takahiko Kojima
INORGANIC CHEMISTRY
(2019)
Article
Chemistry, Multidisciplinary
Wataru Suzuki, Hiroaki Kotani, Tomoya Ishizuka, Takahiko Kojima
CHEMISTRY-A EUROPEAN JOURNAL
(2020)
Correction
Chemistry, Multidisciplinary
Dachao Hong, Takuya Kawanishi, Yuto Tsukakoshi, Hiroaki Kotani, Tomoya Ishizuka, Takahiko Kojima
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
Article
Chemistry, Inorganic & Nuclear
Dachao Hong, Yoshihiro Shimoyama, Yuji Ohgomori, Ryoichi Kanega, Hiroaki Kotani, Tomoya Ishizuka, Yoshihiro Kon, Yuichiro Himeda, Takahiko Kojima
INORGANIC CHEMISTRY
(2020)
Article
Chemistry, Multidisciplinary
Hiroaki Kotani, Hinatsu Shimomura, Kei Ikeda, Tomoya Ishizuka, Yoshihito Shiota, Kazunari Yoshizawa, Takahiko Kojima
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
Article
Multidisciplinary Sciences
Hiroto Fujisaki, Tomoya Ishizuka, Hiroaki Kotani, Yoshihito Shiota, Kazunari Yoshizawa, Takahiko Kojima
Summary: Efficient oxidation of alkanes, especially methane, is essential for using natural gas as chemical feedstock. Current industrial processes use high-temperature and high-pressure steam reforming to generate a gas mixture that can be further converted into products like methanol. However, this study demonstrates a new strategy using N-heterocyclic carbene-ligated Fe-II complexes to capture hydrophobic methane substrate from an aqueous solution, oxidize it to hydrophilic methanol, and release it back into the solution. By increasing the size of the hydrophobic cavities, the effect can be enhanced, achieving a turnover number of 5.0 x 10(2) and a methanol selectivity of 83% during a 3-hour methane oxidation reaction.
Article
Chemistry, Multidisciplinary
Tomoya Ishizuka, Atsushi Hosokawa, Takuya Kawanishi, Hiroaki Kotani, Yipeng Zhi, Takahiko Kojima
Summary: The promise of artificial photosynthesis in solving environmental and energy issues has sparked intensive research into photocatalytic systems for CO2 reduction. This study focuses on a dinuclear Ru-II complex that acts as a self-photosensitizing catalyst, demonstrating high efficiency and durability in CO2 reduction to produce CO.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Tomoya Ishizuka, Taichi Kogawa, Chisato Ogawa, Hiroaki Kotani, Yoshihito Shiota, Kazunari Yoshizawa, Takahiko Kojima
Summary: We synthesized and characterized a Ru-II-OH2 complex and studied its coordination equilibrium and oxidation reaction. The complex exhibits η6 coordination and intramolecular hydrogen bonding, which are important for catalytic oxidation reactions.
Review
Chemistry, Multidisciplinary
Tomoya Ishizuka, Nitika Grover, Christopher J. Kingsbury, Hiroaki Kotani, Mathias O. Senge, Takahiko Kojima
Summary: This article summarizes the synthetic methods and design aspects of nonplanar porphyrin formation, the key properties and functionality of the nonplanar aromatic framework, and the scope and utility of this emerging class in addressing important scientific, industrial, and environmental issues.
CHEMICAL SOCIETY REVIEWS
(2022)
Article
Materials Science, Biomaterials
Haruka Araki, Shota Hagiwara, Ryosuke Shinomiya, Atsuya Momotake, Hiroaki Kotani, Takahiko Kojima, Takuro Ochiai, Naohiko Shimada, Atsushi Maruyama, Yasuhiko Yamamoto
Summary: The study found that the formation of an interpolyelectrolyte complex between heme-DNAzyme and a cationic copolymer with protonated amino groups can enhance the catalytic activity of heme-DNAzyme. This enhancement is attributed to the acid catalysis of protonated amino groups in the polymer, facilitating the formation of Compound I intermediate and improving the activity of heme-DNAzyme. Additionally, the enhancement of heme-DNAzyme activity by the polymer is dependent on factors such as the local heme environment and substrate accessibility to the heme.
BIOMATERIALS SCIENCE
(2021)
Article
Chemistry, Inorganic & Nuclear
Takuya Sawaki, Tomoya Ishizuka, Nanase Namura, Dachao Hong, Mayuko Miyanishi, Yoshihito Shiota, Hiroaki Kotani, Kazunari Yoshizawa, Jieun Jung, Shunichi Fukuzumi, Takahiko Kojima
DALTON TRANSACTIONS
(2020)
Article
Chemistry, Multidisciplinary
Hiroto Fujisaki, Tomoya Ishizuka, Yoshihiro Shimoyama, Hiroaki Kotani, Yoshihito Shiota, Kazunari Yoshizawa, Takahiko Kojima
CHEMICAL COMMUNICATIONS
(2020)
Article
Chemistry, Physical
Hiroaki Kotani, Takuya Miyazaki, Emi Aoki, Hayato Sakai, Taku Hasobe, Takahiko Kojima
ACS APPLIED ENERGY MATERIALS
(2020)
Article
Chemistry, Physical
Amandeep Jindal, Kentaro Tashiro, Hiroaki Kotani, Toshiaki Takei, Sven Reichenberger, Galina Marzun, Stephan Barcikowski, Takahiko Kojima, Yohei Yamamoto
ACS APPLIED ENERGY MATERIALS
(2019)