Article
Chemistry, Inorganic & Nuclear
Priya Singh, Eleanor Stewart-Jones, Melissa C. Denler, Timothy A. Jackson
Summary: High-valent metal-oxo intermediates play a crucial role in oxygen-atom transfer reactions, and changes in metal reduction potential can lead to variations in reaction mechanisms. The rate variations observed for Mn-IV-oxo complexes are primarily controlled by activation enthalpy, indicating a single-step OAT mechanism. This suggests that large variations in sulfoxidation by Mn-IV-oxo centers occur without a change in reaction mechanism.
DALTON TRANSACTIONS
(2021)
Article
Engineering, Chemical
Xiru Chen, Changyin Zhu, Fengxiao Zhu, Guodong Fang, Dongmei Zhou
Summary: Sulfite combined with UV light has been found to efficiently degrade diethyl phthalate (DEP) under aerobic conditions. The study indicates that oxidative radicals, hydrated electron, and hydrogen atom are generated in the sulfite/UV system. Hydrogen atom is the dominant reactive species for DEP degradation. Ethanol and tert-butyl alcohol can promote DEP degradation by quenching the reaction of oxidative radicals. Solution pH and the presence of humic acid greatly affect DEP degradation. It is suggested that H-center dot generated during sulfite/UV process plays an important role in pollutant degradation.
SEPARATION AND PURIFICATION TECHNOLOGY
(2022)
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
Biochemistry & Molecular Biology
Tristan Skipworth, Mardan Khashimov, Iyanu Ojo, Rui Zhang
Summary: In this study, chromium(IV)-oxo porphyrins and chromium(V)-oxo porphyrins were prepared and their reactivities towards thioanisoles were investigated. Chromium(V)-oxo porphyrins exhibited significantly higher reactivity compared to chromium(IV)-oxo species in oxidizing thioanisoles, suggesting them as potent oxidants.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Nitika Pradhan, Antara Garai, Bratati Patra, Sanjib Kar, Prasanta K. Maiti
Summary: The oxo(corrolato)chromium(V) complex selectively kills leukemia cells without inducing cell death in primary non-cancer cells, and the observed cell death in leukemia cells is linked to DNA damage. Interestingly, the DNA in primary cells remained mostly unaffected. DNA from normal and cancerous cell lines exhibited similar trends, and the chemical reductant DTT did not have an additive effect on DNA damage.
CHEMICAL COMMUNICATIONS
(2021)
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
Engineering, Manufacturing
S. Connor Perryman, Mark D. Dadmun
Summary: The study investigates the use of multi-amines to strengthen interlayer adhesion in 3D printed objects by forming covalent bonds between layers. Results show successful formation of covalent bonds and strengthening of the interlayer interface with various multi-amines, with reactions primarily occurring shortly after filament deposition. The research suggests that the aromaticity of the crosslinker plays a key role in creating a stronger interface, providing foundational understanding for applying this protocol to various extrusion-based additive processes and materials.
ADDITIVE MANUFACTURING
(2021)
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
Engineering, Environmental
Changrong Zhao, Bin Liu, Tingting Zhu, Xuewu Zhu, Xiaoxiang Cheng
Summary: This study proposes a novel structure of FeCN membrane that combines membrane technology with photocatalytic and peroxyacetic acid oxidation for the removal of hard-to-degrade organic pollutants from water. The FeCN membrane possesses visible photocatalytic capability and peroxyacetic acid activation, and shows fast degradation of pollutants.
JOURNAL OF HAZARDOUS MATERIALS
(2023)
Article
Engineering, Environmental
Rongrong Liu, Ranxiao Tang, Jizheng Feng, Tao Meng
Summary: Dual-atom catalysts (DACs) have the potential to efficiently regulate multiple reaction pathways and understand the fundamental mechanisms, breaking the limitations of single-atom catalysts (SACs) in heterogeneous catalysis. Fe-DAs/NC with Fe2-N6 moieties was successfully synthesized and employed as an alkaline oxygen reduction reaction (ORR) catalyst. The ORR performances of Fe-DAs/NC were significantly improved compared to single-atom Fe-N4 catalyst due to the synergistic effect of Fe2-N6 moiety.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Katrin Warm, Alice Paskin, Uwe Kuhlmann, Eckhard Bill, Marcel Swart, Michael Haumann, Holger Dau, Peter Hildebrandt, Kallol Ray
Summary: In this study, a novel S=2 oxoiron(IV) species supported by a unique ligand was generated and characterized. This species exhibited high reactivity in hydrogen atom abstraction reactions and demonstrated a unique oxidative mechanism. Complex 2 can serve as an excellent electronic and functional model for biological oxoiron(IV) intermediates.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Robert J. Mayer, Harpreet Kaur, Sophia A. Rauscher, Joseph Moran
Summary: Metal ions can catalyze transamination under biologically relevant conditions, with Cu2+, Ni2+, Co2+, and V5+ identified as the most active. These ions primarily accelerate the reaction by stabilizing key imine intermediates or increasing the acidity of the bound imine. Direct metal ion-catalyzed amino group transfer is highly favored even in the absence of cofactors or protein catalysts under biologically compatible reaction conditions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Tomohiro Higashi, Kazuhiko Seki, Yutaka Sasaki, Yuriy Pihosh, Vikas Nandal, Mamiko Nakabayashi, Naoya Shibata, Kazunari Domen
Summary: This study investigated the HER of Rh nanoparticles coated with an ultrathin layer of Cr-oxides as a model electrode for the Cr2O3/Rh-metal core-shell-type cocatalyst system. The CrOx layer on RhNP facilitated the electron transfer process, leading to increased current density for the HER. It was found that the CrOx layer promoted proton transfer to the RhNP surface and restricted electron transfer from the FTO to the electrolyte and/or RhNP, resulting in efficient photocatalytic water splitting.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Mian Guo, Jisheng Zhang, Lina Zhang, Yong-Min Lee, Shunichi Fukuzumi, Wonwoo Nam
Summary: In this study, six manganese(IV)-oxo complexes bearing electron-rich and -deficient porphyrins were synthesized and investigated in various oxidation reactions. The research found a reversed reactivity between the electron-rich and -deficient Mn(IV)-oxo porphyrins in hydrogen atom transfer and oxygen atom transfer reactions at different temperatures.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Green & Sustainable Science & Technology
Huiyu Liu, Jun Zhang, Jing Gu, Rui Shan, Haoran Yuan, Yong Chen
Summary: Selective upcycling of waste plastics into value-added chemicals is crucial for resource utilization. This study presents a one-pot reaction in methanol to selectively transform polyethylene terephthalate (PET) into arenes (BTX) without the need for external hydrogen supply. The mechanism of hydrogen transfer pathway during the process was elucidated. By using Pt/TiO2 as catalyst, a desirable BTX yield of 77.96% was achieved after 3 hours of reaction.
JOURNAL OF CLEANER PRODUCTION
(2023)
Article
Chemistry, Multidisciplinary
Tomoya Ishizuka, Takahiko Kojima
Summary: This manuscript surveys the synthesis and properties of porphyrin derivatives with fused five-membered rings at the periphery. These derivatives exhibit unique properties, such as expanded aromatic and anti-aromatic circuits passing through the outer rim of the fused rings.
JOURNAL OF PORPHYRINS AND PHTHALOCYANINES
(2023)
Article
Chemistry, Inorganic & Nuclear
Keita Shichijo, Yohei Kametani, Yoshihito Shiota, Kazunari Yoshizawa, Mamoru Fujitsuka, Hisashi Shimakoshi
Summary: A dehydrocorrin complex, Co(II)-pyrocobester (P ( -Co(II) )), was semisynthesized from cyanocobalamin and its photochemical and electrochemical properties were compared to those of the cobester (C ( -Co(II) )). The UV-vis absorptions of P ( -Co(II) ) in CH2Cl2 were red-shifted due to the pi-expansion of the macrocycle in the pyrocobester. The redox couple of P ( -Co(II) ) was positively shifted compared to that of C ( -Co(II) ), coinciding with the high electronegativity of the dehydrocorrin macrocycle. The reactivity of P ( -Co(I) ) was evaluated by its reaction with methyl iodide.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Seiji Ogo, Takeshi Yatabe, Tamon Tome, Riko Takenaka, Yoshihito Shiota, Kenji Kato
Summary: In this study, a homogeneous catalyst is used to synthesize hydrogen peroxide using H2 and O2 in water, eliminating the need for flammable H2/O2 mixtures and cocatalysts. The catalyst is capable of extracting electrons from H2, storing them for the reduction of O2, and then converting the reduced oxygen to H2O2. The catalyst exhibits the highest turnover number (TON) among all homogeneous catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
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, Inorganic & Nuclear
Hideo Nagashima, Yoshihito Shiota, Kazunari Yoshizawa
Summary: Density functional theory calculations verified the reaction pathways of the two catalytic cycles and determined that the modified Chalk-Harrod cycle is more favorable. However, this mechanism contradicts some experimental results, which were resolved by assuming the presence of additional catalysts.
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, Physical
Hiroto Fujisaki, Takahiko Kojima
Summary: This article surveys recent progress in the efficient and selective functionalization of methane using molecular metal complexes as catalysts. The reactions involve C-H bond cleavage by high-valent metal-oxo complexes and C-H bond activation at lower-valent metal centers, resulting in the formation of C-O or C-C bonds through oxygen-rebound, reductive elimination or insertion processes. The importance of hydrophobic environments around metal centers to improve the efficiency and product selectivity of CH4 oxidation is also discussed.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Hiroto Fujisaki, Masaya Okamura, Shiro Hikichi, Takahiko Kojima
Summary: Fe(ii) complexes with pentadentate ligands, including N-heterocyclic carbene moieties, were immobilized onto perfluorinated mesoporous aluminosilicate. These heterogeneous catalysts exhibited excellent performance and selectivity in alkane hydroxylation and cyclohexene epoxidation using H2O2 as the oxidant in CH3CN solvent.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Alexander M. Prophet, Kritanjan Polley, Gary J. Van Berkel, David T. Limmer, Kevin R. Wilson
Summary: The oxidation kinetics of iodide by ozone at the air-water interface is studied in single microdroplets. Molecular simulations and kinetic modeling are used to understand the underlying multiphase mechanism.
Article
Chemistry, Multidisciplinary
Rong Zhang, Jiajing Lan, Fei Wang, Shumei Chen, Jian Zhang
Summary: By utilizing 1,1'-ferrocene dicarboxylic acid as a chelating and surface protection ligand, we have synthesized multi-nuclear indium oxide clusters with varying nuclear sizes, including heptanuclear and thirteen-nuclear clusters. These clusters possess labile coordination sites, allowing for structural modification and self-assembly, resulting in the formation of various cluster structures.
Article
Chemistry, Multidisciplinary
Hui Wang, Hui Liu, Mingsen Wang, Jiaheng Hou, Yongjun Li, Yuancheng Wang, Yingjie Zhao
Summary: Two supramolecular complexes were prepared using CBs and M1, and their single-crystal structures were analyzed by SCXRD. The unexpected 1:2 self-assembly structure between M1 and CB[8] was discovered for the first time. These complexes exhibit unique photophysical properties and provide valuable information about the structure and photophysical properties of supramolecular complexes.
Article
Chemistry, Multidisciplinary
Chang-Hee Lee, Sookil Park, Sanggil Kim, Ji Young Hyun, Hyun Soo Lee, Injae Shin
Summary: The epidermal growth factor receptor (EGFR) is a cell-surface glycoprotein involved in cell proliferation and tumor development. This study used a fluorescently labeled EGFR to investigate its time-dependent endocytosis in live cells and found that appended glycans affect EGFR internalization. Additionally, the study detected sialic acid residues attached to EGFR on the live cell surface using FRET-based imaging. This research provides valuable insights into the cellular functions of EGFR.
Article
Chemistry, Multidisciplinary
Subhankar Sahu, Lokesh Kumar, Sumita Das, Dipti Gupta, Ruchi Anand
Summary: This study proposes a strategy that combines organic electronics with biosensor scaffolds to create a compact device for monitoring environmental aromatic pollution. By coupling biosensing protein MopR with an organic electrochemical transistor (OECT), a sensor module capable of efficient detection of phenol was designed. Exclusive phenol detection with minimal loss of sensitivity could be achieved in complex pollutant mixtures and real environmental samples.
Review
Chemistry, Multidisciplinary
Changseok Lee, Hyung-Joon Kang, Sungwoo Hong
Summary: The formation of C-N bonds through hydroamination reactions catalyzed by nickel hydrides has been a topic of recent interest. This approach offers a way to efficiently transform a variety of alkene and alkyne substrates into compounds enriched with C-N bonds. The review provides a concise overview of the underlying reaction mechanisms and aims to stimulate further progress in NiH-catalytic techniques and catalyst design.
Article
Chemistry, Multidisciplinary
Yueci Wu, Lu-Lu Sun, Hai-Hao Han, Xiao-Peng He, Weiguo Cao, Tony D. James
Summary: Drug-induced liver injury (DILI) is a common cause of acute liver failure in the USA and Europe, but most cases can be recovered or prevented by discontinuing the offending drug. Recent research has found that peroxynitrite (ONOO-) can be used as a potential indicator for early diagnosis of DILI, and there is an urgent need to establish a method to detect and track peroxynitrite in DILI cases. In this study, a FRET-based nano fluorescent probe CD-N-I was developed, which showed high selectivity and sensitivity in detecting peroxynitrite. The probe successfully detected exogenous peroxynitrite in live cells and endogenous peroxynitrite in APAP-induced liver injury of HepG2 cells.
Article
Chemistry, Multidisciplinary
Dmitry L. Lipilin, Mikhail O. Zubkov, Mikhail D. Kosobokov, Alexander D. Dilman
Summary: This article describes a direct photocatalytic method for the thiolation of unprotected acids, which was previously challenging. By using a thionocarbonate reagent with an N-O bond, the efficient conversion of carboxylic acids to thiols is achieved.
Article
Chemistry, Multidisciplinary
Jason Malenfant, Lucille Kuster, Yohann Gagne, Kouassi Signo, Maxime Denis, Sylvain Canesi, Mathieu Frenette
Summary: Raman microscopy can reveal compound-specific vibrational fingerprints without sample preparation. The combination of efficient theoretical calculations and a user-friendly software can accurately predict peak positions and provide match scores to assist with structure determination.
Article
Chemistry, Multidisciplinary
Jayoh A. Hernandez, Paul S. Micus, Sean Alec Lois Sunga, Luca Mazzei, Stefano Ciurli, Gabriele Meloni
Summary: Essential trace metals play crucial roles in the survival and virulence of bacterial pathogens. Helicobacter pylori requires nickel for colonization and persistence in the stomach, and NixA is an essential nickel transporter in this process. This study characterizes the selectivity and electrogenic nature of NixA-mediated nickel transport.
Article
Chemistry, Multidisciplinary
Tarali Devi, Kuheli Dutta, Jennifer Deutscher, Stefan Mebs, Uwe Kuhlmann, Michael Haumann, Beatrice Cula, Holger Dau, Peter Hildebrandt, Kallol Ray
Summary: This study emphasizes the importance of subtle electronic changes and secondary interactions in the stability of biologically relevant metal-dioxygen intermediates. It also shows that the role of the chloride ligand in stabilizing the Fe-III-(OOBu)-Bu-t moiety can extend to other anions, including the thiolate ligand.
Article
Chemistry, Multidisciplinary
Jacqueline R. Santhouse, Jeremy M. G. Leung, Lillian T. Chong, W. Seth Horne
Summary: By studying the folding kinetics and mechanism of the BdpA sequence, researchers found that altering the backbone connectivity can affect protein folding. This suggests that protein mimetic chains have a significant degree of plasticity in transitioning between unfolded and folded states.
Article
Chemistry, Multidisciplinary
Divanshu Gupta, Ralf Einholz, Holger F. Bettinger
Summary: This study presents the first direct spectroscopic evidence of a cyclic seven-membered iminoborane. Compared to linear amino-iminoboranes, this cyclic iminoborane exhibits weakened bond strength and lower Lewis acidity value. The study suggests that the reduced ring strain of cyclic iminoborane prevents nitrogen fixation but allows facile (2 + 2) cycloaddition reaction with C2H4.
Article
Chemistry, Multidisciplinary
Renny Mathew, Aniruddha Mazumder, Praveen Kumar, Julie Matula, Sharmarke Mohamed, Petr Brazda, Mahesh Hariharan, Brijith Thomas
Summary: This study reveals the packing arrangement of partially disordered nitro-perylenediimide (NO2-PDI) using a synergistic approach that combines 3D ED, ssNMR, and DFT techniques. By overcoming these challenges, this methodology opens up new avenues for material characterization, driving exciting advancements in the field.