Article
Chemistry, Physical
Pablo D. Nieres, Victoria A. Vaillard, Juan Zelin, Nicolas I. Neuman, Andres F. Trasarti, Carlos R. Apesteguia, Santiago E. Vaillard
Summary: HG(2) is a reliable and extremely useful catalyst for synthesizing olefins, especially for the self-metathesis reaction of unsaturated fatty acid methyl esters. Silica gel is a promising support for large scale application of HG(2) due to its beneficial characteristics. However, storing the supported catalyst under atmospheric conditions at 298K significantly decreases its activity, which compromises its stability and applicability. Detailed experimental and spectroscopic studies, along with electronic structure calculations, shed light on the catalyst decomposition process.
Review
Chemistry, Physical
Takashi Matsuo
Summary: This review article discusses the application of designed Hoveyda-Grubbs-type complexes in bio-relevant studies, addressing issues and strategies when used in aqueous media, and controlling the reactivities of the complexes through structural modification. It also introduces a recent finding on the ruthenium complex transfer reaction between Hoveyda-Grubbs-type complexes and biomolecules.
Article
Chemistry, Organic
Takashi Matsuo
Summary: Hoveyda-Grubbs-type complexes with ruthenium center coordinated by an N-heterocyclic carbene and a 2-alkoxybenzylidene ligands are important catalysts for olefin metathesis with applications in biochemical research. Structural modification allows for application of these complexes to biomolecules, while studies on the mechanism of olefin metathesis in aqueous media have been conducted.
JOURNAL OF SYNTHETIC ORGANIC CHEMISTRY JAPAN
(2021)
Article
Chemistry, Multidisciplinary
Bengi Ozgun Ozturk, Begum Sariaslan, Mina Askun, Zeynep Tunali, Solmaz Karabulut Sehitoglu
Summary: In this study, a sequential one-pot alkyne dimerization/hydration protocol was developed for the regioselective synthesis of alpha,beta-unsaturated ketones in quantitative yields. The reactions proceeded with high regioselectivity and rapid conversion, producing the corresponding unsaturated ketones within 15 minutes. Different arylacetylene derivatives could be efficiently converted to alpha,beta-unsaturated ketones in quantitative yields using this method.
NEW JOURNAL OF CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Andrej Sterman, Izidor Sosic, Zdenko Casar
Summary: This work describes the preparation and application of primary trifluoroborate-iminiums (pTIMs) as a new and valuable class of organoboron derivatives. Highly enantioselective hydrogenation reactions were used to obtain chiral primary trifluoroborate-ammoniums (pTAMs). A facile conversion method using hexamethyldisiloxane/aqueous HCl was then used to synthesize diverse chiral alpha-aminoboronic acids from chiral pTAMs. The synthesis of optically pure anti-cancer drugs bortezomib and ixazomib demonstrated the practicality of this method.
Article
Chemistry, Multidisciplinary
Jing Gao, Yue Zheng, Wei Yu, Yanan Wang, Tengyu Jin, Xuan Pan, Kian Ping Loh, Wei Chen
Summary: This study demonstrates the use of 2D ferroelectric alpha-In2Se3 as an active channel material to emulate typical synaptic functions. The synaptic device features multimode operations enabled by coupled ferroelectric polarization under various voltage pulses applied at both drain and gate terminals, with energy consumption reduced to around 1 pJ by using high-kappa dielectric. The successful control of ferroelectric polarizations in alpha-In2Se3 and its application in artificial synapses are expected to inspire the implementation of 2D ferroelectric materials for future neuromorphic systems.
Review
Chemistry, Multidisciplinary
Shun Hirota, Satoshi Nagao
Summary: Cytochrome c is a multifunctional water-soluble heme protein that plays important roles in apoptosis and the mitochondrial respiratory chain. Through 3D domain swapping, cytochrome c molecules can form oligomers and polymers. Cytochrome c interacts with cardiolipin on the inner mitochondrial membrane, and its peroxidase activity increases when interacting strongly with cardiolipin.
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN
(2021)
Review
Chemistry, Multidisciplinary
Hulin Tai, Shun Hirota, Sven T. Stripp
Summary: Hydrogenases are metalloenzymes capable of efficiently catalyzing proton reduction and hydrogen oxidation. This Account discusses the use of photochemistry and infrared spectroscopy to study the dynamic hydrogen-bonding changes in [NiFe]- and [FeFe]-hydrogenases, revealing distinct structures and functions in these systems.
ACCOUNTS OF CHEMICAL RESEARCH
(2021)
Article
Biochemistry & Molecular Biology
Satoshi Nagao, Ayaka Idomoto, Naoki Shibata, Yoshiki Higuchi, Shun Hirota
Summary: In this study, metal-binding sites were introduced into proteins using 3D domain swapping, resulting in stable dimeric myoglobins with metal-binding sites. The mutants with specific metal-binding sites showed similarities in spectroscopic properties with wild-type myoglobin. The metal ions bound to the metal-binding sites in the domain-swapped myoglobin dimers exhibited different coordination structures, demonstrating the potential to construct artificial metalloproteins using domain swapping.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2021)
Article
Multidisciplinary Sciences
Masaru Yamanaka, Tsuyoshi Mashima, Michio Ogihara, Mei Okamoto, Takayuki Uchihashi, Shun Hirota
Summary: Ferritin can form a hydrogel from concentrated apoferritin solutions through acid denaturation and subsequent neutralization, with a water content of approximately 80%. The hydrogel exhibits stability and the ability to adsorb and release metal ions, demonstrating a unique property of ferritin as a potential material for future biomaterial design.
Article
Biochemical Research Methods
Takahiro Imanishi, Koji Nishikawa, Midori Taketa, Katsuhiro Higuchi, Hulin Tai, Shun Hirota, Hironobu Hojo, Toru Kawakami, Kiriko Hataguchi, Kayoko Matsumoto, Hideaki Ogata, Yoshiki Higuchi
Summary: This study investigated the binding state of CO with the hydrogenase in Citrobacter sp. S-77 using activity assays, spectroscopic techniques, and X-ray crystallography. The results showed a positive correlation between CO tolerance and oxygen tolerance in [NiFe]-hydrogenases.
ACTA CRYSTALLOGRAPHICA SECTION F-STRUCTURAL BIOLOGY COMMUNICATIONS
(2022)
Review
Chemistry, Multidisciplinary
Sven T. Stripp, Benjamin R. Duffus, Vincent Fourmond, Christophe Leger, Silke Leimkueshler, Shun Hirota, Yilin Hu, Andrew Jasniewski, Hideaki Ogata, Markus W. Ribbe
Summary: Gases like H-2, N-2, CO2, and CO are important feedstock for green energy conversion and as sources of nitrogen and carbon. However, their industrial transformation and production require significant energy input, whereas nature efficiently converts them at ambient conditions using gas-processing metalloenzymes (GPMs). In this review, the importance of the cofactor/protein interface in GPMs is emphasized, and the effects of second and outer coordination sphere on catalytic activity are discussed.
Article
Chemistry, Physical
Mohan Zhang, Hulin Tai, Sachiko Yanagisawa, Masaru Yamanaka, Takashi Ogura, Shun Hirota
Summary: The peroxidase activity of cytochrome c increases when Met80 dissociates from the heme iron, which is related to the initial cyt c membrane permeation step of apoptosis. This study analyzed the resonance Raman spectra of Met80-depleted horse cytochrome c (M80A cyt c) to understand the heme ligand properties of Met80-dissociated cyt c. The results showed that the frequencies of Fe-His stretching and Fe-O2 stretching modes of M80A cyt c were higher than other His-ligated heme proteins, indicating strong heme coordination and the imidazolate character of His18. Moreover, the frequencies of the oxygenated species of M80A cyt c were observed to have a positive linear relationship, suggesting that the Fe-O and O-O bonds are important for the peroxidase activity when Met80 dissociates from the heme iron.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Biochemistry & Molecular Biology
Ibuki Nakamura, Hiroshi Amesaka, Mizuho Hara, Kento Yonezawa, Keisuke Okamoto, Hironari Kamikubo, Shun-ichi Tanaka, Takashi Matsuo
Summary: This study investigates the applicability of synthetic binding proteins, specifically monobodies, in regulating the functions of proteins that undergo large conformational changes. The results show that monobodies can capture and stabilize specific conformational states of proteins, thereby affecting their functions. This suggests that monobody-based modulators can regulate the functions of proteins with significant conformational changes.
Article
Chemistry, Inorganic & Nuclear
Tsubasa Kinugawa, Takashi Matsuo
Summary: This paper investigates the effect of adding chalcogen atoms (sulfur or oxygen) to the benzylidene ligand of the Hoveyda-Grubbs second-generation complex (HG-II) on its catalytic properties. The study shows that the sulfur ligand enhances the stability and methanol tolerance of the catalyst, while the oxygen ligand decreases catalyst durability.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Yuji Mikata, Marin Tanaka, Saori Yasuda, Aya Tsuruta, Taeka Hagiwara, Hideo Konno, Takashi Matsuo
Summary: BQDMEN and its 6-methoxyquinoline derivative (6-MeOBQDMEN) are fluorescent sensors with minor response to Zn2+ and Cd2+. However, when three methoxy substituents are introduced at the 5,6,7-position of the quinoline rings, the fluorescent metal ion selectivity is reversed to favor Cd2+. This reversal of preference is also valid for 1,3-propanediamine derivatives. The dinuclear cadmium complex is suggested to be the key component for the fluorescent Cd2+ selectivity.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Yuji Mikata, Mizuho Uchida, Hinata Koike, Sunao Shoji, Yutaka Ohsedo, Yasushi Kawai, Takashi Matsuo
Summary: Eighteen mononuclear copper(II) complexes with oxygen-containing N4O1 pentadentate ligands were synthesized and the effects of substitution of (iso)quinoline heteroaromatics at different positions on the properties of copper(II) complexes were investigated. The results indicate that the steric hindrance caused by the peri hydrogen atom in quinoline at the Ar-3 position enhances the coordination ability of quinoline nitrogen and ether oxygen atoms to the metal center. The quinoline substitution at the Ar-3 site exhibits an opposite effect compared with those at the Ar-1 and Ar-2 sites in the absorption spectra.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Shun Hirota, Chun-Liang Chiu, Chieh-Ju Chang, Pei-Hua Lo, Tien Chen, Hongxu Yang, Masaru Yamanaka, Tsuyoshi Mashima, Cheng Xie, Hiroshi Masuhara, Teruki Sugiyama
Summary: The spatial and temporal control of amyloid fibril formation of cytochrome c was achieved using a combined method of disulfide bond cross-linking of cysteine-introduced variants and optical trapping. It was identified that the structural change in the region containing Ala83 is essential for amyloid fibril formation.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Inorganic & Nuclear
Yuji Mikata, Minori Kaneda, Shizuka Yonemura, Miyu Akedo, Hideo Konno, Takashi Matsuo
Summary: The selectivity of TQEN towards metal ions was altered by introducing different substituents, with 8-MOMOTQEN showing high selectivity and sensitivity towards Cd2+. The MOMO group played a crucial role in enhancing fluorescent metal-ion selectivity.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Multidisciplinary
Cheng Xie, Hiromitsu Shimoyama, Masaru Yamanaka, Satoshi Nagao, Hirofumi Komori, Naoki Shibata, Yoshiki Higuchi, Yasuteru Shigeta, Shun Hirota
Summary: Research has shown that enhancing the hydrogen bond network at the hinge region can stabilize the structure of myoglobin dimer, further supporting the connection between myoglobin dimer and monomer through 3D domain swapping.
Article
Chemistry, Organic
Takashi Matsuo
Summary: Hoveyda-Grubbs-type complexes with ruthenium center coordinated by an N-heterocyclic carbene and a 2-alkoxybenzylidene ligands are important catalysts for olefin metathesis with applications in biochemical research. Structural modification allows for application of these complexes to biomolecules, while studies on the mechanism of olefin metathesis in aqueous media have been conducted.
JOURNAL OF SYNTHETIC ORGANIC CHEMISTRY JAPAN
(2021)
Review
Chemistry, Multidisciplinary
Dan He, Yawen Li, Fuwen Zhao, Yuze Lin
Summary: High trap density in organic solar cells leads to localized charge carriers and reduced carrier lifetime, limiting device efficiency. This feature article summarizes the recent advances of trap suppression by material design and device engineering.
CHEMICAL COMMUNICATIONS
(2024)
Review
Chemistry, Multidisciplinary
Olivier Monfort, Arshitha Madhusudhan, Martin Motola
Summary: This article presents the advantages of coupling photocatalysis and Fenton-based processes for environmental remediation and discusses their synergy. It critically examines the simultaneous triggering of these two processes and provides insights into research approaches. The study aims to enhance understanding of this complex process and highlight the potential integration of new catalysts in current wastewater treatment technology.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Manideepa Dhar, Chittaranjan Mishra, Avijit Das, Uttam Manna
Summary: An approach of 'polymerization of monomers in its aggregated form' has been introduced to tailor the water wettability of fibrous and porous substrates, achieving hydrophobicity to superhydrophobicity transition, as well as patterned wettability. This facile chemical method provides a durable coating with adjustable and patterned wettability for various potential applications.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Saswat Ranjan Bhoi, Chhanda Debnath, Shikha Gandhi
Summary: In this article, a novel catalytic reaction using Pd(0) and Bronsted acid is reported for the synthesis of biologically important imidazolidinone-fused N-heterocycles through redox-neutral intramolecular N-allylation of indoles and pyrroles with alkynes. This atom-economical method is applicable to a wide range of substrates and eliminates the need for leaving groups or oxidizing agents commonly used in traditional allylation reactions.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Longkun Chen, Mingshuai Zhang, Meichen Liu, Zhuoyuan Liu, Yuetong Qiu, Zhilai Zhang, Fuchao Yu, Jiuzhong Huang
Summary: In this study, an efficient Rh(III)-catalyzed selective mono- and dual-C-H bond functionalization/cyclization with iodonium ylide as the sole coupling partner was demonstrated. Fused benzodiazepine skeletons were obtained in excellent yields, providing an improved approach to dual C-H unsymmetrical functionalization.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Alice Kennett, Sven Epple, Gabriella van der Valk, Irene Georgiou, Evelyne Gout, Romain R. Vives, Angela J. Russell
Summary: This study presents the design and synthesis of sulfated disaccharide inhibitors based on IdoA(2S)-GlcNS(6S), which showed potent inhibition of Sulf-2. The results suggest that IdoA(2S)-GlcNS(6S) is the shortest fragment size required for effective inhibition of Sulfs, and a trisulfated disaccharide is identified as the minimal fragment size of heparan sulfate for effective endosulfatase inhibition.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Mauro Garbini, Andrea Brunetti, Riccardo Pedrazzani, Magda Monari, Massimo Marcaccio, Giulio Bertuzzi, Marco Bandini
Summary: The self-adaptability of galvanostatic electrolysis was found to be helpful in a multistage chemo- and diastereoselective electrochemically promoted cyclodimerization of chalcones. Through a series of reductive events, densely functionalized cyclopentanes with five contiguous stereocenters were obtained (25 examples, yields up to 95%, dr values up to >20:1). Further experimental and electrochemical investigations indicated the crucial role of dynamic kinetic resolution of the aldol intermediate in the reaction mechanism.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Dhananjay S. Nipate, Neha Meena, Prakash N. Swami, Krishnan Rangan, Anil Kumar
Summary: In this study, the synthesis of functionalized benzo[a]phenazines and indazolo[2,3-a]quinolines was achieved through Rh(III)-catalyzed oxidative annulation of 2-arylquinoxalines and 2-aryl-2H-indazoles with allyl alcohols. The method showed a wide substrate scope, excellent functional group tolerance, good to high yields of annulated products, and the capability for scaled-up synthesis. A tentative mechanism of the annulation reaction was proposed based on a preliminary mechanistic investigation.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Ruonan Zhang, Abudukadi Tudi, Xia Yang, Xuping Wang, Zhihua Yang, Shujuan Han, Shilie Pan
Summary: A new lead tellurium borate material with a unique fundamental building block [B4O10] was synthesized and found to exhibit high birefringence. The structure-property relationship was discussed using first-principles calculations.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Amresh Kumar Singh, Baishali Thakurta, Anupam Giri, Monalisa Pal
Summary: This study introduces three key concepts for the quick synthesis of large-scale high-quality 2D materials films and their utilization in device fabrication.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Reina Hagiwara, Shun Nishimura, Kosuke Okeyoshi
Summary: A copolymer-conjugated nanocatalytic system has been developed to improve electron transfer and enhance photoinduced H2 generation.
CHEMICAL COMMUNICATIONS
(2024)
