Article
Chemistry, Multidisciplinary
Kritika Keshari, Moumita Bera, Lucia Velasco, Sandip Munshi, Geetika Gupta, Dooshaye Moonshiram, Sayantan Paria
Summary: A terminal (FeOH)-O-III complex has been synthesized and characterized, showing the formation of a ligand radical complex in further reactions mimicking the oxygen rebound step of cytochrome P450. Kinetic analysis revealed the crucial role of a hydrogen atom transfer mechanism in the reactions.
Article
Chemistry, Multidisciplinary
Philip Netzsch, Regina Stroh, Florian Pielnhofer, Ingo Krossing, Henning A. Hoeppe
Summary: Borosulfates offer fascinating structures and properties beyond pure silicate analogy. Mg-3[H2O -> B(SO4)(3)](2) is the first borosulfate with a boron atom coordinated by three tetrahedra, exhibiting higher Lewis and Brønsted acidity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Correction
Chemistry, Inorganic & Nuclear
Guangjian Liao, Fuming Mei, Zhuqi Chen, Guochuan Yin
Summary: In this study, the improvement of tryptophan 2,3-dioxygenase activity for olefin oxygenation by a non-heme iron(II) complex was achieved through the introduction of a Lewis acid, showing promising catalytic performance.
DALTON TRANSACTIONS
(2022)
Article
Biochemistry & Molecular Biology
Arun Dhaka, Olivier Jeannin, Emmanuel Aubert, Enrique Espinosa, Marc Fourmigue
Summary: The ability of alkylseleno/alkyltelluroacetylenes to act as a ditopic chalcogen bond donor in co-crystals with ditopic Lewis bases is extended to the octafluorobiphenylene analog, demonstrating a shorter and more linear C-Se...N ChB interaction in the 1:1 co-crystal compared to the previous counterpart.
Article
Engineering, Environmental
Tielong Li, Chaolin Gao, Wei Wang, Yaxin Teng, Xiao Li, Haitao Wang
Summary: By increasing the degree of substitution (D.S.) of CMC, this study successfully reversed the negative influence of CMC on the properties of S-nZVI, resulting in higher longevity and ee. CMC with super high D.S. showed compatible molecular structure and significantly enhanced the properties of S-nZVI.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Byung Heung Park, Hun Yong Shin, Bong-Seop Lee
Summary: The electropositivity of carbon atom in CO2 allows it to act as a proton acceptor or electron acceptor in Lewis acid-base interactions with organic chemicals. High-pressure CO2/alcohol solvent systems are vital for supercritical extraction, dehydration of alcohols, and extraction of natural products. Understanding the Lewis acid-base interactions between CO2 and alcohols is crucial for the solvation process under high-pressure conditions and the development of thermodynamic models.
JOURNAL OF CO2 UTILIZATION
(2021)
Article
Chemistry, Inorganic & Nuclear
T. Ilgin Demirer, Bernd Morgenstern, Diego M. Andrada
Summary: The synthesis, structure, and bonding analysis of phosphanylgallane with P-H and Ga-Cl/H substitution are reported in this study. Lewis base- and Lewis acid/base-stabilized monomeric phosphanylgallane derivatives were obtained by reacting with LiPHR or LiPHR(BH3). These findings are of significance for studying the properties and applications of this class of compounds.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Yasutaka Tsuji, Kazumasa Kon, Takahiro Horibe, Kazuaki Ishihara
Summary: A chiral amidophosphate-N-iodosuccinimide cooperative catalysis has been developed for the site-, diastereo-, and enantioselective iodocyclization of 2-geranylarenols with molecular iodine to give iodo-containing polycyclic compounds with good selectivity. The catalytic system involves the formation of a reactive chiral iodonium species through dual halogen-bonding interactions with a chiral Lewis base and Lewis acid. The bulky 3,3'-substituents of the chiral BINOL-derived amidophosphate are crucial for inducing site-selective iodination at the less-hindered terminal alkenyl moiety of 2-geranylarenols.
CHEMISTRY-AN ASIAN JOURNAL
(2023)
Article
Engineering, Environmental
Zhixiao Liu, Zaixu An, Zhiming Mi, Zihan Wang, Qian Zhu, Dexing Zhang, Junman Wang, Jing Liu, Jialiang Zhang
Summary: Developing nano-filtration (NF) membranes with high permeance and high rejection is crucial for addressing water pollution and scarcity. The novel NF membranes with PAO as organic interlayer exhibited outstanding desalination performance, with a rejection above 99% for Na2SO4 and a permeance up to 25.2 L/m(2) h bar.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2022)
Article
Chemistry, Multidisciplinary
Chang-Quan Wu, Yi-Wen Wu, Xuan-Han He, Ruo-Ting Hong, Hao-Chien Lee, Kang-Yen Feng, Peter Ping-Yu Chen
Summary: This study investigates the effect of saddle-shaped deformation on the reaction of Fe-III hemes with hydrogen peroxide. The results show that greater saddle deformation in Fe-III porphyrins can enhance the orbital interaction with the O-O bond, facilitating O-O cleavage. The study provides insights into the catalytic mechanism of this reaction.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Biochemistry & Molecular Biology
Chamila P. Manankandayalage, Daniel K. Unruh, Ryan Perry, Clemens Krempner
Summary: The Lewis acid-base adducts of general formula X(nad)<-NC5H4-C5H4N->B(nad)X [nad = 1,8-O2C10H6, X = C6H5 (2c), 3,4,5-F3-C6H2 (2d)] were synthesized and characterized. H-shaped adduct 2d formed stable host-guest complexes with aromatic hydrocarbon solvents. Crystallographic analysis revealed pi...pi interactions between the adduct and solvents, resulting in 1:1 and 1:2 host-guest complexes. The complexes demonstrated high thermal stability. The ability of 1,8-dihydroxy naphthalene to self-assemble through dative covalent N -> B bonds was demonstrated.
Article
Chemistry, Physical
Xiaoxue Sun, Qinghua Wang, Shenghan Wu, Xinyu Zhao, Ligang Wei, Kunlan Li, Jingai Hao, Li Wei, Shangru Zhai, Qingda An
Summary: Ammonia is considered a promising hydrogen or energy carrier, and its absorption or adsorption is crucial for ammonia removal, storage, and separation applications. Metal-containing deep eutectic solvents (DESs) have shown excellent ammonia absorption performances, with MgCl2/Res/EG (0.1:1:2) DES outperforming other reported DESs. The outstanding NH3 absorption properties of metal-containing DESs are attributed to the synergy of Lewis acid-base and hydrogen bonding interactions.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Inorganic & Nuclear
Wanjie Ren, Charles E. Schulz, Mark H. Shroyer, Wei Xu, Shibo Xi, Pengfei An, Wenping Guo, Jianfeng Li
Summary: In this study, the electronic configurations of (nitrosyl)iron corroles with different para-substituted phenyl groups were investigated. Various techniques were employed to characterize these complexes and determine their electronic and magnetic properties. The study also established correlations between the electronic characteristics of the para-substituents and the electrochemical behavior and magnetic parameters of the complexes.
INORGANIC CHEMISTRY
(2022)
Article
Biochemistry & Molecular Biology
Hai T. Dong, Yu Zong, Abigail J. Bracken, Michael O. Lengel, Jeff W. Kampf, Debangsu Sil, Carsten Krebs, Nicolai Lehnert
Summary: Flavodiiron NO reductases (FNORs) are important enzymes in microbial pathogenesis, and the second coordination sphere (SCS) hydrogen bond network is critical for the NO reduction reaction catalyzed by FNORs. A model complex of FNORs with pendant hydrogen bond donors was synthesized, and a strategy to stabilize mononitrosyl diiron complexes using the SCS was discovered.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2022)
Article
Chemistry, Physical
J. F. Carstens, J. Bachmann, G. Guggenberger
Summary: This study found that electrostatic attraction rather than hydrophilic repulsion controlled the aggregation and transport behavior of soil mineral colloids. The irregular shape and surface roughness of the colloids rendered the short-range hydrophilic repulsion ineffective, allowing the more long-range electrostatic interactions to predominate.
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
(2021)
Article
Chemistry, Physical
Aram Manukyan, Harutyun Gyulasaryan, Armen Kocharian, Paul Oyala, Ratibor Chumakov, Marina Avramenko, Carlos Sanchez, Oscar O. Bernal, Lusegen Bugaev, Eduard Sharoyan
Summary: Carbon microspheres composed of nanographene and amorphous carbon were synthesized using the solid-phase pyrolysis method. Nitrogen and carbon atoms were incorporated into the graphene lattice as pyrrolic and pyridinic coordination. The sample exhibited strong paramagnetism and ferromagnetism, attributed to the presence of edge states and nitrogen impurity atoms.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Heejun Lee, Jun Myun Ahn, Paul H. Oyala, Cooper Citek, Haolin Yin, Gregory C. Fu, Jonas C. Peters
Summary: Photoinduced, copper-catalyzed couplings of nitrogen nucleophiles with alkyl electrophiles have been shown to be an attractive approach for achieving enantioselective C-N bond formations. This study provides mechanistic insight into a previously reported photoinduced, copper-catalyzed enantioconvergent C-N coupling. Experimental and computational results support the proposed intermediates and their chemical stability and competence in producing the desired C-N coupling product with enantioselectivity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Hyungdo Cho, Hidehiro Suematsu, Paul H. Oyala, Jonas C. Peters, Gregory C. Fu
Summary: Transition-metal catalysis of substitution reactions of alkyl electrophiles by nitrogen nucleophiles is an important strategy for synthesizing higher-order amines and controlling their stereochemistry. This study reports the photo-induced enantioconvergent coupling of racemic tertiary alkyl electrophiles with aniline nucleophiles using a readily accessible chiral copper catalyst. The mechanism of this catalytic process has been elucidated using various tools, leading to the identification of key copper-based intermediates in the proposed cycle.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Dirk J. Schild, Lucie Nurdin, Marc-Etienne Moret, Paul H. Oyala, Jonas C. Peters
Summary: This study reports the generation and low temperature characterization of a terminally bound iron(III) nitride, which is proposed as an intermediate in iron-mediated nitrogen fixation. Electron spin resonance spectroscopy and DFT calculations reveal the electronic structure of this nitride species, with the majority of the spin residing on boron.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Inorganic & Nuclear
Angela A. Shiau, Heui Beom Lee, Paul H. Oyala, Theodor Agapie
Summary: This article reports the synthesis and characterization of a stable (Mn4O4)-O-IV cuboidal complex supported by a disiloxide ligand. The substitution of an anionic acetate or amidate ligand with a dianionic disiloxide ligand improves the stability and shifts the reduction potential of the complex.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Maryann Morales, Raheleh Ravanfar, Paul H. Oyala, Harry B. Gray, Jay R. Winkler
Summary: The first encoded protein of SARS-CoV-2, Nsp1, binds to the human 40S ribosome and inhibits the synthesis of host proteins, thereby suppressing the innate immune response. The last 33 residues of the unstructured C-terminus of Nsp1 adopt a specific geometric structure upon binding to the ribosome.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Mackenzie J. Field, Paul H. Oyala, Michael T. Green
Summary: Experimental data and theoretical calculations have shown an inverse correlation between oxygen spin population and electron donation from the axial ligand, indicating its crucial role in the reactivity of C-H bond cleavage.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Pablo Garrido-Barros, Matthew J. Chalkley, Jonas C. Peters
Summary: While research on synthetically catalyzed nitrogen reduction (N2R) to produce ammonia is extensive, the catalysis of producing hydrazine (N2H4) has been less explored, although it has considerable mechanistic interest. This study revealed that irradiation of a tris(phosphine)borane (P-3(B)) Fe catalyst significantly increased the production of N2H4 instead of NH3, contrary to its usual high selectivity for NH3. The key factor determining selectivity is identified as a terminal hydrazido intermediate (P3Fe)-Fe-B=NNH2, which undergoes protonation to release NH3 in its singlet ground state, while a low-lying triplet excited state leads to reactivity at N-alpha and formation of N2H4.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Inorganic & Nuclear
Brendon J. McNicholas, Cherish Nie, Anex Jose, Paul H. Oyala, Michael K. Takase, Larry M. Henling, Alexandra T. Barth, Alessio Amaolo, Ryan G. Hadt, Edward I. Solomon, Jay R. Winkler, Harry B. Gray, Emmanuelle Despagnet-Ayoub
Summary: Thirteen boronated cyanometallates and one metalloboratonitrile have been characterized and studied for their electronic structures and redox properties. The results showed that these compounds exhibit highly reversible redox couples and some of them are surprisingly stable.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
David A. Cagan, Daniel Bim, Brendon J. McNicholas, Nathanael P. Kazmierczak, Paul H. Oyala, Ryan G. Hadt
Summary: In this study, a facile photochemical method was used to generate a library of Ni(I)-bpy halide complexes and their relative reactivity was evaluated. Structure-function relationships were established to rationalize the ligand-controlled reactivity towards high energy and challenging C(sp(2))-Cl bonds. The mechanism of formal oxidative addition was found to proceed through an SNAr-type pathway, which contrasts the mechanism observed for weaker C(sp(2))-Br/I bonds.
INORGANIC CHEMISTRY
(2023)
Article
Biochemistry & Molecular Biology
Ji Huang, Xiangyang Liu, Yadong Sun, Zhuang Li, Min-Han Lin, Keith Hamilton, Corey R. Mandel, Felix Sandmeir, Elena Conti, Paul H. Oyala, Liang Tong
Summary: Human cleavage and polyadenylation specificity factor (CPSF)73, which catalyzes the cleavage reaction for the 3'-end processing of pre-mRNAs, contains a mixture of metal ions, including Fe, Zn, and Mn, in its active site. The abundance of these metal ions varies in samples prepared from different expression hosts. Zinc plays a critical role in the nuclease activity of CPSF73 and its homolog INTS11 for RNA 3'-end processing.
JOURNAL OF BIOLOGICAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Angela A. Shiau, Heui Beom Lee, Paul H. Oyala, Theodor Agapie
Summary: This study reports the synthesis, crystal structure, electrochemistry, SQUID magnetometry, and EPR spectroscopy of a (MnMnIV)-Mn-III O-3(4) cuboidal complex featuring five-coordinate Mn-III. The cluster displays a spin ground state of S = 5/2, while conversion to a six-coordinate Mn upon treatment with water results in a spin state change to S = 1/2. These results demonstrate that coordination number has a substantial effect on spectroscopy, even without dramatic changes within the Mn4O4 core.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Inorganic & Nuclear
Abigail J. Bracken, Hai T. Dong, Michael O. Lengel, Nicolai Lehnert
Summary: Recent research on Flavodiiron nitric oxide reductases (FNORs) has revealed their role in providing pathogens with resistance to immune defense agent nitric oxide (NO). Understanding the mechanism of how FNORs mediate NO reduction contributes to the development of new therapeutic approaches against drug-resistant strains.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
M. Jeremy Amdur, Kathleen R. Mullin, Michael J. Waters, Danilo Puggioni, Michael K. Wojnar, Mingqiang Gu, Lei Sun, Paul H. Oyala, James M. Rondinelli, Danna E. Freedman
Summary: In this study, the researchers have improved the relaxation time of molecular qubits by controlling the orbital angular momentum and ligand rigidity, providing guidelines for designing new qubit candidates operating at high temperatures.
Article
Chemistry, Multidisciplinary
Luciano Barluzzi, Nadir Jori, Tianyi He, Thayalan Rajeshkumar, Rosario Scopelliti, Laurent Maron, Paul Oyala, Theodor Agapie, Marinella Mazzanti
Summary: This study reports the first example of a transition metal-capped uranium nitride, which forms a UMo interaction with Mo(0) and shows reactivity towards CO oxidation.
CHEMICAL COMMUNICATIONS
(2022)