Article
Chemistry, Multidisciplinary
Gloria Tobajas-Curiel, Qingqing Sun, Jeremy K. M. Sanders, Pablo Ballester, Christopher A. Hunter
Summary: Molecular recognition in water involves various factors such as polar functional group interactions, desolvation of polar and non-polar surfaces, and changes in conformational flexibility. Supramolecular complexes that can be studied in both water and non-polar solvents are used to dissect the effects of substituents on aromatic interactions. The study reveals that H-bonding interactions and aromatic interactions contribute significantly to the stability of the complex, with substituents further enhancing the stability.
Article
Chemistry, Inorganic & Nuclear
Gracjan Kurpik, Anna Walczak, Mateusz Goldyn, Jack Harrowfield, Artur R. Stefankiewicz
Summary: A wide range of functionalized pyridine ligands have been used to synthesize various Pd(II) complexes with different structures. The functionalization of ligand molecules has a significant impact on the physicochemical properties of the coordination compounds. The study also reveals the relationship between NMR chemical shifts and ligand basicity. Furthermore, weak interactions have been identified through detailed crystallographic analysis, which explains the solution chemistry of the complexes. These Pd(II) complexes show efficient and versatile catalytic activity in Suzuki-Miyaura and Heck cross-coupling reactions.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Sharmila Samaroo, Charley Hengesbach, Chase Bruggeman, Nunzio Giorgio G. Carducci, Lincoln Mtemeri, Richard J. J. Staples, Thomas Guarr, David P. P. Hickey
Summary: This article investigates the correlation between the solubility of N-substituted pyridinium salts in a non-aqueous solvent and the C-H...p interactions. It finds a direct correlation between the two, highlighting the significant impact of minimal structural changes on pyridinium solubility.
Article
Chemistry, Analytical
N. G. S. Mateyise, M. M. Conradie, J. Conradie
Summary: A series of bis(tpy)ruthenium(II) complexes with different substituents were synthesized, and their electrochemical properties were studied experimentally and theoretically. The results showed that the electronic donating/withdrawing nature of the substituents can be quantitatively measured by Hammett constants, and can be used to design complexes with desired oxidation or reduction potential. Moreover, these complexes were found to have potential applications as dye sensitizers in dye-sensitized solar cells.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Cristina A. Barboza, Pawel Gawrys, Marzena Banasiewicz, Boleslaw Kozankiewicz, Andrzej L. Sobolewski
Summary: This study investigated the impact of electron acceptor/donor group substitution on the photophysical properties of TSANs through spectroscopic techniques and ab initio quantum chemistry methods. The results confirmed the dependence of multiple emission bands on the substitution of electron donating and accepting groups, and revealed new differences in the phosphorescence behavior of TSANs.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Zafar Mahmood, Jia He, Shuqing Cai, Zhanxiang Yuan, Hui Liang, Qian Chen, Yanping Huo, Burkhard Koenig, Shaomin Ji
Summary: This study demonstrates the tuning of the redox potential and excited state properties of a commercially available photocatalyst for the visible-light-mediated photoredox phosphorylation of tertiary aliphatic amines. It also showcases the successful synthesis of alpha-aminophosphinoxides and alpha-aminophosphonates through cross-dehydrogenative coupling reactions using Ru-II complexes as photocatalysts.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Binzhou Lin, Hao Liu, Ishwor Karki, Erik C. Vik, Mark D. Smith, Perry J. Pellechia, Ken D. Shimizu
Summary: Stabilizing nitrogen pnictogen bond interactions were measured using molecular rotors. Intramolecular C=O···N interactions were formed in the bond rotation transition states which lowered the rotational barriers and increased the rates of rotation, as measured by EXSY NMR. The pnictogen interaction energies show a very strong correlation with the positive electrostatic potential on nitrogen, which was consistent with a strong electrostatic component. In contrast, the NBO perturbation and pyramidalization analyses show no correlation, suggesting that the orbital-orbital component is minor. The strongest C=O···N pnictogen interactions were comparable to C=O···C=O interactions and were stronger than C=O···Ph interactions, when measured using the same N-phenylimide rotor system. The ability of the nitrogen pnictogen interactions to stabilize transition states and enhance kinetic processes demonstrates their potential in catalysis and reaction design.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biochemistry & Molecular Biology
Qiang Zhao
Summary: The regium-pi stacking interactions in the Au-6⋯PhX complexes were studied, and it was found that the effects of electron-donating and electron-withdrawing substituents on the interactions are different. Moreover, the interactions between substituted benzene and Au-6 cluster were found to be stronger compared to the Au-6⋯benzene complex.
JOURNAL OF MOLECULAR MODELING
(2021)
Article
Chemistry, Multidisciplinary
Alexander K. Mengele, Dominik Weixler, Avinash Chettri, Maite Maurer, Fabian Lukas Huber, Gerd M. Seibold, Benjamin Dietzek, Bernhard J. Eikmanns, Sven Rau
Summary: The research revealed that ligand design can control the mechanism of photooxidation. One of the Ru(II) complexes, Rudppz, enabled efficient turnover through supramolecular binding to facilitate cofactor oxidation, allowing repetitive conversion of naturally occurring nicotinamides by recognizing the redox state of the cofactor.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Ian Colliard, May Nyman
Summary: M-IV molecular oxo-clusters, such as Ce-70, have diverse crystal structures and can form intricate frameworks with divalent transition metals and Ce-monomer linkers. These clusters show potential for catalysis, ion exchange, and oxidation-reduction reactions, opening up new possibilities for metal-organic framework design.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Kun Zhang, Zewen Jiang, Fanghua Ning, Biao Li, Huaifang Shang, Jin Song, Yuxuan Zuo, Tonghuan Yang, Guang Feng, Xinping Ai, Dingguo Xia
Summary: Understanding the anionic redox behavior with respect to metal-ligand interactions in Li-rich oxide cathodes is crucial for developing high-capacity battery materials. By analyzing the orbital combinations of transition metals and oxygen in LROs, it was found that a pi-type oxygen redox mode can be achieved at low voltages, expanding the fundamental theories of anionic redox and providing a new design route for high-capacity cathode materials. The interaction between oxygen and central Rh in Li2RhO3 demonstrates high reactivity in the occupied anti-bonding state, showing a novel low-voltage oxygen redox mechanism.
ADVANCED ENERGY MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Michio Yamada
Summary: This article summarizes recent advances in experimental and theoretical efforts to characterize the nature and strength of non-covalent interactions on fullerene surfaces. The studies include host-guest chemistry based on various macrocycles, catalyst chemistry based on conjugated molecular catalysts, and conformational isomerism analyses using fullerene-based molecular torsion balances and computational chemistry. These studies have provided a comprehensive evaluation of the contributions of electrostatic, dispersion, and polar interactions on the surface of fullerenes.
Article
Chemistry, Multidisciplinary
Nicole Houszka, Hannes Mikula, Dennis Svatunek
Summary: 1,2,4,5-Tetrazines are widely used in bioorthogonal chemistry for their high reactivity in Diels-Alder reactions. The substituents in the 3- and 6-positions of the tetrazine scaffold significantly affect the rate of cycloadditions, but this is not explained by frontier molecular orbital interactions. Instead, the high reactivity of mono-substituted tetrazines is due to decreased Pauli repulsion, leading to a more asynchronous approach and reduced distortion energy. Additionally, ethylene is not a good model compound for other alkenes in Diels-Alder reactions.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Marcus Korb, Stephen A. Moggach, Paul J. Low
Summary: An unusual 1,2-ferrocenyl migration was observed after reactions of [Ru(dppe)Cp][BAr4F] with diferrocenylacetylene, expanding the scope of group rearrangments beyond methyl and phenyl entities. Bimetallic bis(vinylidene) complexes were formed from ferrocene-containing bis(alkynes) following two consecutive rearrangements.
CHEMICAL COMMUNICATIONS
(2021)
Article
Chemistry, Organic
Guilherme L. Kosteczka, Rafael N. Soek, Wagner E. Richter, Renan B. Campos
Summary: This study explores the competitive formation of isomeric bridged lactams via acid-catalyzed intramolecular Schmidt reactions from 3-azidoethylcyclopentanones using density functional theory (DFT) calculations. The results indicate that specific substituents at alpha-carbons can efficiently control the reaction's regioselectivity through lone pair-cation interactions or steric hindrance, while cation-pi interactions are less effective.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2023)
Article
Chemistry, Analytical
Wataru Tadano, Eishi Tanabe, Jens R. Stellhorn, Kenji Komaguchi, Shinjiro Hayakawa
Summary: A commercial X-ray CT apparatus was used to estimate and compare the density of fragmented single fibers using a quasi-monochromatic beam. The quasi-monochromaticity of the X-ray source was validated through radiograph measurements. Increasing the number of averaged voxels in the 3D-CT image improved the statistical quality. The CT values of the polymers showed a good relationship with their density, and an analytical curve derived from measurements of reference samples could accurately determine the relative density of unknown fragmented fibers. The coefficient of variation of the estimated density ranged from 1.5% to 2%. Furthermore, the correlation of CT values was better with the linear absorption coefficient than with density.
ANALYTICAL SCIENCES
(2023)
Article
Chemistry, Multidisciplinary
Ndaru Candra Sukmana, Sugiarto, Jun Shinogi, Tatsuhiro Kojima, Akifumi Higashiura, Akima Yamamoto, Takemasa Sakaguchi, Masahiro Sadakane
Summary: By solid-state heating of methylammonium monomolybdate, (CH3NH3)2[MoO4], in air, methylamine and water are released to form (CH3NH3)6[Mo7O24] and (CH3NH3)8[Mo10O34], which eventually transform into MoO3. We present the first single-crystal X-ray structural analysis of (CH3NH3)2[MoO4] and (CH3NH3)6[Mo7O24], showing that the decamolybdate structure is different from that of ammonium molybdates. Moreover, (CH3NH3)6[Mo7O24] serves as an effective negative staining reagent for transmission electron microscopy of viruses, such as SARS-CoV-2 and influenza virus.
Article
Chemistry, Multidisciplinary
Ayman H. Zaki, Nao Tsunoji, Yusuke Ide
Summary: Researchers modified the synthesis conditions to obtain green rust materials with controlled properties and discovered a sample with excellent solar photocatalytic activity for hydrogen production.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Esmail Doustkhah, Nao Tsunoji, M. Hussein N. Assadi, Yusuke Ide
Summary: In order to maximize the surface-to-body ratio, it is necessary to use smaller metallic palladium nanoparticles for catalytic applications. However, if the supported palladium is below a critical size, the hybridization with the supporting material can decrease the labile electrons that are crucial for catalytic reactions. It has been demonstrated that palladium with at least six atomic layers on silicate sheets exhibits a metallic-like electronic property, resulting in excellent catalytic activity compared to isotropic palladium nanoparticles and single-atom palladium.
ADVANCED MATERIALS INTERFACES
(2023)
Article
Chemistry, Physical
Karen Silva Vargas, Jeremie Zaffran, Marcia Araque, Masahiro Sadakane, Benjamin Katryniok
Summary: The Deoxydehydration (DODH) of glycerol to allyl alcohol was studied over a ceria-supported rhenium oxide catalyst. Mesoporous ceria materials were synthesized using a nanocasting process. The catalyst based on nanocasting ceria showed higher performance with up to 88% yield in allyl alcohol and was reusable for 3 cycles without reactivation step. XPS characterization of the catalyst revealed the presence of Re4+ species after the reaction, which suggested the involvement of two redox couples, Re7+/Re5+ and Re6+/Re4+, during the DODH reaction.
MOLECULAR CATALYSIS
(2023)
Article
Chemistry, Multidisciplinary
Masahiro Sugiarto, Masahiro Sadakane
Summary: This study provides the first single-crystal X-ray structural evidence of the existence of α-H2P2W12O48 potassium salt and discovers two dimeric and one trimeric structures that it forms in solution. These phosphotungstate anions were synthesized through recrystallization of (NH4)12[α-H2P2W12O48] in alkaline solutions. The study also confirms that selective crystallization of these compounds can be achieved through the selection of appropriate counterions and pH values.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Inorganic & Nuclear
Sugiarto, Jun Shinogi, Masahiro Sadakane
Summary: Through 1H NMR spectroscopy analysis, we identified three distinct Cp*Ir-containing tungsten oxide clusters formed in aqueous mixtures of [(Cp*IrCl)2(mu-Cl)2] and Na2WO4 with varying molar ratios. These species were isolated as Na4[(Cp*Ir)2(mu-OH)3]2[(Cp*Ir)2H2W8O30], [(Cp*Ir)2(mu-OH)3]2[(Cp*Ir)2{Cp*Ir(OH2)}2H2W8O30], and [(Cp*Ir)2{Cp*Ir(OH2)}2{Cp*Ir(OH2)2}2H2W8O30](NO3)2. The results indicate that the octatungstate [H2W8O30]10- anion is the main polyoxotungstate species in the presence of {Cp*Ir}2+ cations, which can bind up to six {Cp*Ir}2+ cations on its surfaces. Moreover, the coordination environment of {Cp*Ir}2+ can be altered by coordinating with pyridine.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Tugce Ustunel, Yusuke Ide, Sarp Kaya, Esmail Doustkhah
Summary: Green H2 generation through layered materials, such as layered titanates, plays a significant role in (photo)catalysis due to their high theoretical surface area. In this study, exfoliated few-layer sheets of titanate were successfully obtained by dilute HCl treatment without organic exfoliating agents. Sn single atoms were then loaded onto the exfoliated titanate, resulting in enhanced photocatalytic activity for H2 evolution. The optimized Sn-loaded exfoliated titanate exhibited better performance than conventional TiO2-based photocatalysts.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Takuo Minato, Masahiro Sadakane
Summary: A cationic metal glue strategy utilizing lacunary-type polyoxometalates (POMs) as rigid multidentate ligands is demonstrated for increasing the size and nuclearity of hetero-multinuclear metal-oxo clusters. The method enabled the synthesis of {(FeMn4)Mn2Ln2(FeMn4)} oxo clusters (Ln=Gd, Tb, Dy, and Lu), which are currently the largest reported paramagnetic hetero-multinuclear metal-oxo clusters in POMs.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Qiangqiang Tong, Chuntian Qiu, Guijin Zheng, Qianqian Zhu, Shiman Zhou, Yukang Wang, Li Shi, Huifei Wang, Dingbing He, Masahiro Sadakane, Yanshuo Li, Zhenxin Zhang
Summary: A zeolitic octahedral metal oxide based on niobate (ZOMO-NbOx) with high acidity was synthesized and used as an efficient catalyst for the degradation of fluoroquinolone antibiotics under visible light. The presence of higher acidity promoted the adsorption of ciprofloxacin (CIP) on ZOMO-NbOx, expanding its light-absorbing range from UV to visible light through ligand to metal charge transfer. ZOMO-NbOx exhibited significantly higher catalytic activity compared to commercial Nb2O5, with a TOF value 53 times higher, and remained stable after multiple reuses. It also demonstrated good resistance to inorganic ions and humic acids, and effectively degraded CIP in various natural freshwater bodies. The intermediate products were identified and degradation pathways were proposed.
APPLIED CATALYSIS A-GENERAL
(2023)
Article
Materials Science, Multidisciplinary
Shufan Yao, Yihang Hua, Qianqian Zhu, Qingqing Liu, Bolun Yu, Masahiro Sadakane, Yanshuo Li, Wataru Ueda, Zhenxin Zhang
Summary: Zeolitic octahedral metal oxides based on vanadotungstate show potential in gas separation. The microporosity of these materials can be precisely tuned through structure and composition, influencing their separation performance. In this study, zeolitic vanadotungstate was used for the separation of ethylene and ethane, with Cu as the cation. The Cu-based material exhibited differentiated adsorption performance and high theoretical selectivity, effectively separating the two gases even under harsh conditions.
ADVANCED MATERIALS TECHNOLOGIES
(2023)
Article
Materials Science, Ceramics
Naoki Tarutani, Miki Asanome, Kenji Okada, Masahide Takahashi, Takuo Minato, Masahiro Sadakane, Kiyofumi Katagiri, Kei Inumaru
Summary: Additive manufacturing by vat-photopolymerization is an important technique due to its availability, low cost, low energy consumption, and high-speed printing. This paper reports the synthesis of highly concentrated nanocolloids of nickel hydroxide acrylate and their use in vat-photopolymerization. By adding a small quantity of organic cross-linker, bulky objects can be formed.
JOURNAL OF THE CERAMIC SOCIETY OF JAPAN
(2023)
Article
Chemistry, Inorganic & Nuclear
Qingqing Liu, Shufan Yao, Denan Li, Baokai Ma, Tianyi Zhang, Qianqian Zhu, Dingbing He, Masahiro Sadakane, Yanshuo Li, Wataru Ueda, Zhenxin Zhang
Summary: The redox-triggered microporosity change in zeolitic iron molybdate is investigated, and it is found that the micropores of the material can be adjusted by redox reactions, enabling tuning of the adsorption and separation performance.
INORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Analytical
Hiroki Ishida, Naoki Yamasaki, Yuuki Otsuka, Daichi Mori, Tomoko Shimamura, Takuya Hasegawa, Shuhei Ogo, Tadaharu Ueda
Summary: An on-site electrochemical antioxidant capacity measurement system was developed and compared with spectroscopic methods and conventional electrochemical methods. The system showed promising results and was able to measure the antioxidant capacities of various antioxidants and vegetable extracts quickly and accurately.
ANALYTICAL SCIENCES
(2022)
Article
Chemistry, Multidisciplinary
Naoya Nakano, Maki Torimoto, Hiroshi Sampei, Reiji Yamashita, Ryota Yamano, Koki Saegusa, Ayaka Motomura, Kaho Nagakawa, Hideaki Tsuneki, Shuhei Ogo, Yasushi Sekine
Summary: This study investigates the effect of an electric field on the dry reforming of methane. The results show that the application of an electric field significantly enhances the conversion rate of methane and carbon dioxide, and promotes the reaction between surface oxygen and methane at the Pt and CeO2 interface.
