Article
Chemistry, Inorganic & Nuclear
Yuji Mikata, Yuri Aono, Chihiro Yamamoto, Hiromi Nakayama, Arimasa Matsumoto, Fukue Kotegawa, Masafumi Harada, Hajime Katano, Yoshio Kobayashi, Sachiko Yanagisawa, Minoru Kubo, Atsushi Kajiwara, Masahito Kodera
Summary: In this study, a bis(mu-oxo)diiron(IV,IV) complex was synthesized as a model for intermediate Q in the methane monooxygenase reaction cycle. The structure of the complex was characterized by X-ray crystallography and spectroscopic techniques, and its high reactivity was demonstrated through hydrogen abstraction reactions.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Tho Huu Le, Phu Hoang Dang, Hai Xuan Nguyen, Truong Nhat Van Do, Nhan Trung Nguyen, Mai Thanh Thi Nguyen
Summary: Four new stilbene-like derivatives were isolated from the stems of Streblus ilicifolius, and Streblus E exhibited potent tyrosinase inhibitory activity. Molecular docking study revealed that Streblus E had lower binding affinity for oxy-tyrosinase compared to Streblus C.
Article
Chemistry, Multidisciplinary
Gayea Hyun, Mihui Park, Gwangmin Bae, Jong-woan Chung, Youngjin Ham, Seonyong Cho, Seungwon Jung, Suhwan Kim, Yong Min Lee, Yong-Mook Kang, Seokwoo Jeon
Summary: The effects of homogenized triple-phase boundaries (TPBs) on reaction kinetics in air cathodes with structurally designed pore networks are explored. The diffusion fluxes of reactants are visualized by modeling, revealing evenly distributed reaction areas within the periodic open structure. Homogeneous TPBs in cathode structural engineering provide a new strategy for improving reaction kinetics in Li-O2 batteries.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Adrian-Alexandru Somesan, Richard A. Varga
Summary: A new family of C,O-chelating aryl ligands, 2-(ROCH2)C6H4, R = Me, Pr-i, Bu-t, was introduced to the low-valent organolead chemistry, resulting in the successful synthesis of homoleptic plumbylenes and corresponding hexaaryldiplumbanes.
NEW JOURNAL OF CHEMISTRY
(2022)
Article
Engineering, Environmental
Zhi Xu, Zi-He Meng, Song-Hai Wu, Shi-Jie Wang, Peng-Yue Zhu, Yong Liu, Hai-Tao Ren, Shao-Yi Jia, Xu Han
Summary: This study reveals that both Cu(III)-peroxo species and SO4 center dot- play important roles in the oxidation of As(III) in the Cu(II)-S(IV) system, enriching our understanding of the diversity of oxidizing species in metal-S(IV) systems under alkaline conditions.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Astronomy & Astrophysics
Yurina Nakazato, Naoki Yoshida, Daniel Ceverino
Summary: Recent observations by the James Webb Space Telescope have discovered high-redshift galaxies with strong emission lines from doubly ionized oxygen. Using multiline diagnostics, combined with observations of far-infrared lines, we investigate the physical conditions of the interstellar medium in these galaxies. Our study using the FirstLight simulation suite shows that massive galaxies with stellar masses greater than 10^9 solar masses rapidly evolve chemically to z = 9. We find that young stellar populations in star-forming galaxies enhance the [O iii] line emission, resulting in higher line luminosity to star formation rate ratios compared to low-redshift galaxies.
ASTROPHYSICAL JOURNAL
(2023)
Article
Chemistry, Inorganic & Nuclear
Samuel A. Brunclik, Adedamola A. Opalade, Timothy A. Jackson
Summary: Synthetic manganese catalysts that activate hydrogen peroxide are used for hydrocarbon oxidation reactions. Understanding the decay pathways of different manganese alkylperoxo complexes can help elucidate the factors that affect the O-O cleavage reaction. By using density functional theory calculations and comparing with experimental data, the differences in decay pathways of two different manganese alkylperoxo complexes were rationalized based on their electronic structures.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Fei Yu, Haoyuan Yin, Xueting Bai, Junyao Pan, Xiaochen Zhang, Jie Ma
Summary: In this study, porous carbon/Cu@Cu2O composites derived from MOFs were synthesized and used as cathode materials for capacitive deionization. The materials exhibited excellent desalting capacity and cycle stability, making them a promising choice for capacitive deionization.
CHINESE CHEMICAL LETTERS
(2023)
Article
Chemistry, Inorganic & Nuclear
Matthew J. Evans, Mathew D. Anker, Martyn P. Coles
Summary: The aluminyl anion K[Al(NONDipp)] engages in oxidative additions with the E-H bonds regardless of their polarity, forming (hydrido)aluminate salts. All products were characterized by various spectroscopic techniques and single-crystal X-ray diffraction, highlighting the versatility of aluminyl anions in activating various types of E-H bonds.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Shawn M. Moore, Chen Sun, Jennifer L. Steele, Ellen M. Laaker, Arnold L. Rheingold, Linda H. Doerrer
Summary: There is a strong interest in MnOHx moieties due to the stepwise changes in O-H bonds with Mn oxidation state changes. The reactivity of aquo-derived ligands, {MOHx}, is influenced by the electronic character of other ligands. Preparation of mononuclear Mn complexes with all O-donors is rare despite oxygen coordination being prevalent in biological systems.
Article
Engineering, Environmental
Ying Liu, Wei Miao, Yong Feng, Xian Fang, Qiuju Li, Ningjie Du, Dandan Wang, Shun Mao
Summary: A composite catalyst was prepared with Cu-based metal organic framework (Cu-MOF) derived Cu nanoparticles decorated in a three-dimensional reduced graphene oxide (3D RGO) network, which showed high catalytic activity for 2,4-dichlorophenol (2,4-DCP) degradation in a wide pH range and achieved high mineralization ratio within a short time. The Cu/RGO catalyst exhibited high reactivity toward aromatic compounds with hydroxyl and chlorinated groups.
JOURNAL OF HAZARDOUS MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Wenjuan Zhu, Semin Jang, Jin Xiong, Roman Ezhov, Xiao-Xi Li, Taeyeon Kim, Mi Sook Seo, Yong-Min Lee, Yulia Pushkar, Ritimukta Sarangi, Yisong Guo, Wonwoo Nam
Summary: In this study, a mononuclear non-heme iron(III)-peroxo complex was synthesized and characterized, showing high nu(O-O) value and unprecedented electrophilic reactivity in oxidation reactions. Various spectroscopic techniques confirmed the unique properties of the complex, including its H atom abstraction and O atom transfer reactivity. Additionally, interesting observations were made in the oxidation of benzaldehyde derivatives, indicating the complex's potential in various oxidation reactions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Inorganic & Nuclear
Rui Liu, Yanyan Tang, Chenfeng Wang, Zheng-Feng Zhang, Ming-Der Su, Yan Li
Summary: The reactivities of o-carborane-fused silylenes towards molecules with CE (E = C, P) bonds were studied. Reactions of [(LSi:)C]2B10H10 (1a) with arylalkynes resulted in the formation of bis(silylium) carborane adducts 2 and 3. On the other hand, the reaction of 1a with a phosphaalkyne AdCP led to the synthesis of compound 4, featuring fused CPSi rings with a C=Si double bond and Si-Si single bond. Furthermore, the reaction of monosilylene 1b with AdCP yielded compound 5, containing a 1,2,3-triphosphetene core. The structures of the products were characterized by NMR spectroscopy and/or X-ray crystallography.
INORGANIC CHEMISTRY
(2023)
Article
Multidisciplinary Sciences
Dhruba P. Poudel, Amrit Pokhrel, Raj Kumar Tak, Majji Shankar, Ramesh Giri
Summary: In this paper, a simple photoredox-catalyzed intermolecular cyclopropanation of unactivated alkenes with active methylene compounds is reported. The reaction proceeds in neutral solvent under air or dioxygen with a photoredox catalyst excited by blue light-emitting diode light and an iodine co-catalyst. Mechanistic investigations reveal that photosensitized O-2 plays a vital role in the reaction.
Article
Astronomy & Astrophysics
Yi Hang Valerie Wong, Poya Wang, Tetsuya Hashimoto, Toshinobu Takagi, Tomotsugu Goto, Seong Jin Kim, Cossas K. -W. Wu, Alvina Y. L. On, Daryl Joe D. Santos, Ting-Yi Lu, Ece Kilerci-Eser, Simon C. -C. Ho, Tiger Y. -Y. Hsiao
Summary: The distant galaxy A1689-zD1, discovered through gravitational lensing, offers an important opportunity to study galaxy formation in the early universe. This study detected emission lines and measured redshift, providing insights into the spatial variation and potential physical reasons behind it. The findings shed light on the merging nature of A1689-zD1 and the possibility of obscured regions in the galaxy.
ASTROPHYSICAL JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Laia Vicens, Giorgio Olivo, Miquel Costas
Summary: This study presents a supramolecular strategy for enzyme-like H2O2 activation at a biologically inspired manganese catalyst, allowing for catalytic asymmetric epoxidation. Modulation of both amino acid and catalyst structure can tune the efficiency and enantioselectivity of the reaction, and an investigation on the oxidative degradation pathway of the system is provided.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Johann B. B. Kasper, Pattama Saisaha, Maurits de Roo, Mitchell J. J. Groen, Laia Vicens, Margarida Borrell, Johannes W. W. de Boer, Ronald Hage, Miquel Costas, Wesley R. R. Browne
Summary: This study elucidates the mechanism and reactive species involved in the oxidation of alkenes and alcohols with H2O2 under the presence of a specific catalyst. The findings suggest that a certain reactive species can engage in both alkene and alcohol oxidation reactions, exhibiting selectivity.
Article
Chemistry, Inorganic & Nuclear
Mainak Mitra, Alexander Brinkmeier, Yong Li, Margarida Borrell, Arnau Call, Julio Lloret Fillol, Michael G. Richmond, Miquel Costas, Ebbe Nordlander
Summary: Two new tetradentate N4 ligands and their corresponding Fe(II) complexes have been synthesized and characterized. The complexes exhibit excellent catalytic activity in the hydroxylation of alkanes and the oxidation of cyclooctene, using hydrogen peroxide as oxidant. Isotope labeling experiments provide insight into the steric influence exerted by the ligands on the relative reactivity of the oxo ligands.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Physical
Arnau Vicens, Laia Vicens, Giorgio Olivo, Osvaldo Lanzalunga, Stefano Di Stefano, Miquel Costas
Summary: Site-selective oxidation of aliphatic C-H bonds is achieved using a manganese oxidation catalyst equipped with two 18-benzo-6-crown ether receptors. The catalyst shows excellent selectivity towards the central methylenic sites of the long chain tetradecane-1,14-diamine. This selective oxidation overcomes challenges associated with differentiating between similar sites in organic molecules.
FARADAY DISCUSSIONS
(2023)
Article
Nanoscience & Nanotechnology
Miguel Sanchez-Fuente, Alberto Lopez-Magano, Alicia Moya, Ruben Mas-Balleste
Summary: Condensation of BINAPO-(PhCHO)(2) and 1,3,5-tris(4-aminophenyl)benzene(TAPB) leads to a new imine-based chiral organic material (COM) that can be post-functionalized through reductive transformation of imine linkers to amines. Although the imine-based material is not stable enough to be used as a heterogeneous catalyst, the reduced amine-linked framework can be efficiently utilized in asymmetric allylation of various aromatic aldehydes. The obtained yields and enantiomeric excesses are comparable to those observed for the molecular BINAP oxide catalyst, with the added advantage of recyclability offered by the amine-based material.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Biochemistry & Molecular Biology
Pau Font, Nikolaos V. Tzouras, Argyro T. Papastavrou, Georgios C. Vougioukalakis, Xavi Ribas
Summary: The Lewis-acidic nature and robustness of NHC-Au(I) complexes make them highly effective catalysts for various reactions involving polyunsaturated substrates. Recently, the use of external oxidants or catalysts with pendant coordinating groups has allowed for exploration of Au(I)/Au(III) catalysis. In this study, N-heterocyclic carbene (NHC)-based Au(I) complexes with and without pendant coordinating groups were synthesized and characterized, and their reactivity in the presence of different oxidants was investigated. The results showed that the NHC ligand was oxidized to form NHC=O azolone products when iodosylbenzene-type oxidants were used, and quantitative recovery of gold in the form of Au(0) nuggets was achieved. The synthesized Au(0) nuggets were characterized to have purities above 90% using SEM and EDX-SEM. This study challenges the perceived robustness of the NHC-Au bond and presents a novel methodology for producing Au(0) nuggets.
Article
Chemistry, Physical
Johann B. Kasper, Laia Vicens, C. Maurits de Roo, Ronald Hage, Miquel Costas, Wesley R. Browne
Summary: Mononuclear MnII oxidation catalysts with aminopyridine-based ligands achieve high TON enantioselective epoxidation of alkenes with H2O2. The electronic effect of peripheral ligand substituents plays a role in the enantioselectivity and maximum TON. The use of low temperatures and slow addition of H2O2 reduces competing H2O2 disproportionation and improves TONs for alkene oxidation.
Article
Chemistry, Multidisciplinary
Fabian M. Steudel, Ernest Ubasart, Luigi Leanza, Miriam Pujals, Teodor Parella, Giovanni M. Pavan, Xavi Ribas, Max von Delius
Summary: This study demonstrates the successful synthesis of a challenging task by adding two unsymmetric malonate esters to Buckminster fullerene C60, resulting in 22 spectroscopically distinguishable isomeric products. By combining three different approaches, namely tether approach, template approach, and shadow mask approach, the researchers achieved 87% selectivity for the formation of a single isomer.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Judith Sala, Lorena Capdevila, Cristina Berga, Araceli de Aquino, Laura Rodriguez, Silvia Simon, Xavi Ribas
Summary: In this study, a stepwise synthesis of new nanographenes and polycyclic aromatic hydrocarbons (PAHs) via Scholl ring fusion is reported. The aromatic homologation compounds, obtained through one-step Ni-catalysed Csp2-F functionalization, are shown to be valid precursors for the Scholl reaction. Furanol-bearing PAHs are described for the first time by screening experimental conditions. DFT calculations provide mechanistic insights into the formation of furanol PAHs under moderately acidic conditions. All synthesized PAHs and nanographenes exhibit moderate/weak fluorescent properties, and the crystallized PAHs show some degree of curvature and are obtained as racemic mixtures. Enantiomeric separation of one furanol-bearing PAH allows for the study of its chiroptical CD properties.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Arnau Call, Giorgio Capocasa, Andrea Palone, Laia Vicens, Eric Aparicio, Najoua Choukairi Afailal, Nikos Siakavaras, Maria Eugenia Lopez Salo, Massimo Bietti, Miquel Costas
Summary: This research report presents a simple and general method for the synthesis of chiral γ-lactones through enantioselective oxidation of nonactivated primary and secondary C(sp(3))-H bonds in readily available carboxylic acids. The use of robust sterically encumbered manganese catalysts allows for outstanding enantioselectivities (up to >99.9%) and yields (up to 96%) using hydrogen peroxide as the oxidant. The resulting γ-lactones are of immediate interest for the preparation of natural products and recyclable polymeric materials.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Sergio Sisti, Marco Galeotti, Filippo Scarchilli, Michela Salamone, Miquel Costas, Massimo Bietti
Summary: A detailed study on C(sp(3))-H bond oxygenation reactions catalyzed by [Mn(OTf)(2)((TIPS)mcp)] complex was conducted, showing that the introduction of electron-withdrawing functional groups in different solvents significantly increased site-selectivity and product yield. The study also achieved selective control over multiple methylenic sites.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Andrea Palone, Guillem Casadevall, Sergi Ruiz-Barragan, Arnau Call, Siilvia Osuna, Massimo Bietti, Miquel Costas
Summary: This study describes a catalytic enantioselective hydroxylation method of tertiary C-H bonds in cyclohexane scaffolds using an evolved manganese catalyst and H2O2. The catalytic system provides structural complementarity to the substrate similarly to lock-and-key recognition in enzymatic active sites. Theoretical calculations reveal that enantioselectivity is determined by the precise fitting of the substrate scaffold into the catalytic site through a network of complementary weak non-covalent interactions. Stereoretentive C(sp(3))-H hydroxylation results in the generation of multiple stereogenic centers in a single step, which can be orthogonally manipulated to obtain a variety of chiral scaffolds from a single precursor molecule.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Review
Chemistry, Physical
Miguel Sanchez-Fuente, Jose Lorenzo Alonso-Gomez, Laura M. Salonen, Ruben Mas-Balleste, Alicia Moya
Summary: This review provides an overview of the development of chiral porous organic frameworks as candidates for heterogeneous asymmetric organocatalysis. The synthetic strategies, characterization techniques, and applications of chiral organic materials in asymmetric organocatalysis are summarized. Various types of porous organic frameworks are described, and strategies for incorporating chirality in these materials are presented. The review focuses on the applications of chiral porous organic frameworks in asymmetric organocatalytic reactions, summarizing and categorizing the available literature in the field.
Article
Chemistry, Multidisciplinary
Ashleigh M. Chester, Celia Castillo-Blas, Roman Sajzew, Bruno P. Rodrigues, Ruben Mas-Balleste, Alicia Moya, Jessica E. Snelson, Sean M. Collins, Adam F. Sapnik, Georgina P. Robertson, Daniel J. M. Irving, Lothar Wondraczek, David A. Keen, Thomas D. Bennett
Summary: This study explores the characterization of hybrid blends comprising a metal-organic framework (MOF) glass and a phosphate glass. The mechanical and thermal properties of the blends are studied, and the interfacial interactions between the phases are analyzed.
Article
Chemistry, Multidisciplinary
Ashleigh M. Chester, Celia Castillo-Blas, Roman Sajzew, Bruno P. Rodrigues, Ruben Mas-Balleste, Alicia Moya, Jessica E. Snelson, Sean M. Collins, Adam F. Sapnik, Georgina P. Robertson, Daniel J. M. Irving, Lothar Wondraczek, David A. Keen, Thomas D. Bennett
Summary: This study explores the characterization of hybrid blends comprising a metal-organic framework (MOF) glass and a phosphate glass. The mechanical and thermal properties of the blends are studied, and the interfacial interactions between the phases are analyzed.
