Article
Chemistry, Multidisciplinary
Gyeongjin Park, Francois P. Gabbai
Summary: This study focuses on the hydrogen bonding interaction between a metallobasic gold(I) center and an OH functionality, demonstrating the authentic interaction between them. Moreover, experimental results suggest that increasing the acidity of the OH functionality may not necessarily enhance the stability of the Au(I)···H-O interaction.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Electrochemistry
I. Pacheco, M. Bouvier, O. M. Magnussen, P. Allongue, F. Maroun
Summary: In this study, ultrathin crystalline films of cobalt oxides were grown on Au(111) substrate by electrodeposition. The structure and morphology of the films were investigated, and the influence of the substrate on the morphology of Co3O4 films was studied.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Li Zhao, Piaoping Yang, Song Shi, Guozhi Zhu, Xiao Feng, Weiqing Zheng, Dionisios G. Vlachos, Jie Xu
Summary: Activation of molecular oxygen for selective alcohol oxidation is achieved using a heterogeneous ligand method to prepare a high-efficiency vanadium carbon catalyst. Chemisorbed oxygen and pentavalent vanadium oxide are found to be crucial for catalyst performance. The V-C catalyst activates molecular oxygen to singlet oxygen or its analogue and carries out the reaction through C-H bond activation. The catalyst also shows high efficiency in selectively oxidizing hydroxyl groups in other substrates, providing guidance for the development of nonprecious metal catalysts for aerobic oxidation.
Article
Chemistry, Multidisciplinary
Bin Li, Blaise L. Geoghegan, Christoph Woelper, George E. Cutsail, Stephan Schulz
Summary: This study systematically investigates the reactivity of beta-diketiminate zinc complexes with the redox-active 2,2'-bipyridine. The results show that bpy can serve as a neutral ligand, a p-radical anion, or a diamagnetic dianion in different reactions with LZnI, NaB(C6F5)(4), and KC8. The electronic structure of the complexes is elucidated through various experimental and theoretical methods, revealing the collaborative role of the beta-diketiminate co-ligand and bpy ligand in stabilizing the energy of the LUMO.
Article
Chemistry, Physical
Cesar Ruiz-Zambrana, Macarena Poyatos, Eduardo Peris
Summary: A gold complex with a naphthalene-di-imide-functionalized N-heterocyclic carbene (NHC) ligand was prepared and its reversible redox properties and catalytic activity in the hydroamination of terminal alkynes were studied.
Article
Chemistry, Physical
Conghao Yi, Zuyun He, Yizhang Hu, Dengmin Liang, Yongqing Zhang, Yan Chen
Summary: This study introduces FeOOH@MoS2 as a highly effective and stable activator for peroxymonosulfate (PMS)-based AOPs system, showing exceptional performance in removing antibiotics from aquatic environments under both acidic and basic conditions. The strong catalytic activity of MoS2 as a co-catalyst and the interaction between MoS2 and FeOOH contribute to its high performance and stability. The production and reduction of Fe enable the recyclability of the catalyst, providing a simple strategy to improve the efficiency and stability of heterogeneous Fe-based catalysts in AOP systems, particularly in basic environments, for large-scale implementation.
SURFACES AND INTERFACES
(2021)
Article
Nanoscience & Nanotechnology
Qilei Yang, Qi Li, Xiyang Wang, Xiao Wang, Lei Li, Xuefeng Chu, Dong Wang, Jishuai Men, Xinbo Li, Wenzhe Si, Yue Peng, Yongliang Ma, Junhua Li
Summary: This article presents a novel high-performance diesel oxidation catalyst (DOC) with high steam resistance and thermal stability. By modifying the surface physicochemical environment of CeO2-SmMn2O5, the catalyst exhibits excellent low-temperature oxidation catalytic activity and NO conversion.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Jianhong Su, Yuncong Luo, Xin Xu
Summary: An efficient and selective benzylic C(sp(3))-H addition of o-CH3-substituted tertiary aromatic amines to alkenes has been achieved using a scandium catalyst supported by an anilido-oxazoline ligand, providing an atom-economic method for the synthesis of a new family of alkylated tertiary anilines. A wide range of amine and alkene substrates are compatible with the catalyst system.
CHEMICAL COMMUNICATIONS
(2021)
Article
Chemistry, Inorganic & Nuclear
Si-Jia Guan, Peng Zhang, Shen-Jing Ji, Yu Cao, Nian-Tzu Suen
Summary: The presence of iron impurities in nickel-based electrocatalysts affects the oxygen evolution reaction (OER). Internal iron is found to facilitate phase transformation and improve OER performance.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Huafeng Li, Wenjing Chen, Zelong Yuan, Yuzhen Jin, Yujie Zhao, Pengtao Ma, Jingyang Niu, Jingping Wang
Summary: Three Ru-induced structural interconversion polyoxometalates were synthesized and characterized. The catalytic performances of these compounds in oxidative coupling reactions were found to be strongly dependent on the element contents of the active sites. Compound 1 showed highly efficient photocatalysis, compound 2 exhibited relatively poor efficiency, and compound 3 had no significant contribution to the coupling reaction.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Masazumi Tamura, Eiji Sagawa, Akira Nakayama, Yoshinao Nakagawa, Keiichi Tomishige
Summary: The hybrid catalyst of CeO2 and 2-cyanopyridine is effective in oxidizing alkanes with high selectivity to alcohols and ketones, with the mechanism attributed to the N atom in the CN group playing a key role on the CeO2 surface.
Article
Chemistry, Multidisciplinary
Jessica R. Wilson, Matthias Zeller, Nathaniel K. Szymczak
Summary: In this study, a series of nickel(ii) tris(2-pyridylmethyl)amine (TPA) complexes with appended hydrogen bonds to halides (F, Cl, Br) were synthesized and characterized. Reduction to the nickel(i) state resulted in an unusual nickel(i) fluoride complex stabilized by H-bonds, allowing for structural and spectroscopic characterization.
CHEMICAL COMMUNICATIONS
(2021)
Article
Chemistry, Inorganic & Nuclear
Hashini N. K. Herath, Austin L. L. MacRae, Angel Ugrinov, Glenn R. R. Morello, Alexander R. R. Parent
Summary: Two phosphorus-containing ruthenium complexes were synthesized and characterized spectroscopically and electrochemically. Both complexes exhibited proton-coupled electron transfer (PCET) behavior. A Ru(V/IV) couple was detected at 1.4 V vs. NHE for [Ru(bpyPO(3)H(2))(bpy)Cl]Cl. The complexes were tested for their ability to catalyze C-H bond oxidation and it was found that [Ru(bpyPO(3)H(2))(bpy)Cl]Cl can oxidize secondary C-H bonds using NaIO4 as the primary oxidant under aqueous conditions.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Kei Ikeda, Kazunari Yoshizawa, Yoshihito Shiota
Summary: The benzene hydroxylation catalyzed by ruthenium-substituted Keggin-type polyoxometalates was investigated, showing high chemoselectivity and the heteroatom effect on the reaction's activation free energy. Replacing Si with other elements can significantly affect the efficiency of the catalyst for benzene hydroxylation.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Xiaohan Ye, Chenhuan Wang, Shuyao Zhang, Qi Tang, Lukasz Wojtas, Minyong Li, Xiaodong Shi
Summary: This study achieved enantioselective, intermolecular alkene arylamination through gold redox catalysis. Chiral P,N ligands were found to be the optimal choice, enabling alkene aminoarylation with good yields and excellent stereoselectivity. As the first example of enantioselective gold redox catalysis, this work confirmed the feasibility of applying a chiral ligand at the gold(I) stage and introduced a new way to conduct gold redox catalysis with stereochemistry control.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Elishua D. Litle, Francois P. Gabbai
Summary: This study reports on the formation process of M -> C-carbenium bonds in a series of Group 10 complexes and confirms their dative nature through combined experimental and computational studies.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Inorganic & Nuclear
Mohammadjavad Karimi, Francois P. Gabbai
Summary: This study reports the synthesis and photoreduction of a complex featuring a tetravalent platinum center connected to a germyl ligand. In the presence of a chlorine trap, the complex undergoes a clean photolysis to produce two different products, which were confirmed and quantified using NMR spectroscopy and GC-MS analysis.
Article
Chemistry, Inorganic & Nuclear
M. Karimi, F. P. Gabbai
Summary: To enhance the fluoride binding ability of Lewis acidic stiboranes, a Sb-V derivative has been synthesized and characterized. The derivative features diarylamine groups positioned near the antimony center, allowing for hydrogen bonding interactions with Sb-bound fluoride anions. Experimental and computational results demonstrate that the fluoride ion affinity of this derivative is superior to other compounds.
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
(2022)
Article
Chemistry, Multidisciplinary
Wei-Chun Liu, Francois P. Gabbai
Summary: In this study, we synthesized a tetrafluoroborate salt and found that it can function as a fluorescent fluoride anion sensor. Through spectroscopic and computational analysis, we revealed the mechanism behind the color change, and further investigated the properties of the system through electrochemical studies.
CANADIAN JOURNAL OF CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Mohammadjavad Karimi, Elishua Litle, Francois P. Gabbai
Summary: In this study, gold complexes with halogermanes as ligands were synthesized and investigated. Experimental and computational analyses revealed the presence of an Au -> Ge interaction in these complexes. Chloride abstraction reactions were also studied, and a putative dication was formed by double chloride abstraction with AgSbF6. This dication showed higher catalytic activity than its monocationic analog in alkyne hydroamination reactions.
ISRAEL JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Elishua D. Litle, Francois P. Gabbai
Summary: In this study, two compounds were synthesized to investigate the interaction of gold with fluorenyl cation. Computational results showed that one of the compounds possesses a strong Au -> C+ bond and can effectively activate enyne compounds.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Francois P. Gabbai, Jesse E. Smith
Summary: As part of our investigations into the Lewis acidic behavior of antimony derivatives, we studied the properties of 5-phenyl-5,5-dichloro-lambda 5-dibenzostibole (1), a dichlorostiborane with an antimony atom confined to a five-membered heterocycle. Our work confirmed that the geometric constraints of this compound enhance the Lewis acidity of the antimony atom, as evidenced by crystal structure analysis and solution studies. The compound's enhanced Lewis acidic properties were also observed in pnictogen bonding catalysis experiments involving imine reductions.
Article
Chemistry, Multidisciplinary
Wei-Chun Liu, Francois P. Gabbai
Summary: We have described a new gold chloride complex with an ambiphilic phosphine/xanthylium ligand, in which the AuCl interacts with the pi(+) surface of the xanthylium unit. Energy decomposition analyses on a model system revealed the dominance of non-covalent interactions, particularly electrostatic and dispersion terms. The presence of these AuCl-pi(+) interactions correlates with the high catalytic activity of the complex in various cyclisation reactions.
Article
Chemistry, Multidisciplinary
Benyu Zhou, Francois P. Gabbai
Summary: This study investigates the reaction of O-2 with two distibines in the presence of an ortho-quinone, resulting in the formation of tetraolate complexes. The formation process involves oxidation of the antimony atoms to the +V state and the formation of an alpha,alpha,beta,beta-tetraolate ligand that bridges the two antimony(V) centers. Under aerobic conditions, the tetraolate complexes react with O-2 to form semiquinone/peroxoantimony intermediates and then evolve into bis(antimony(V)) alpha,alpha,beta,beta-tetraolate complexes. The controlled protonolysis and reduction of the bis(antimony(V)) alpha,alpha,beta,beta-tetraolate complexes regenerate the starting distibine and ortho-quinone, producing two equivalents of water as the product of O-2 reduction.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Yunyi Wang, Aili Fan, Ryan D. Cohen, Guilherme Dal Poggetto, Zheng Huang, Haifeng Yang, Gary E. Martin, Edward C. Sherer, Mikhail Reibarkh, Xiao Wang
Summary: The authors developed a practical iHMBC methodology using accurate isotope shift measurement to distinguish two-bond from long-range HMBC correlation. iHMBC can be used as a complement to conventional 2D NMR experiments for determining multiple bond heteronuclear correlations in small to medium-sized organic molecules.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Logan T. Maltz, Francois P. Gabbai
Summary: We present the findings of a computational study on the binding of fluoride by various pentavalent pnictogen Lewis acids. Through activation strain and energy decomposition analyses, we identified the electrostatic and orbital contributions to these acid-base interactions, as well as the significance of Pauli repulsion and molecular flexibility in determining relative Lewis acidity among the pnictogens. Our results highlight antimony-based species as the strongest fluoride binders, and emphasize the importance of Pauli repulsion and molecular flexibility in determining this relative Lewis acidity.
INORGANIC CHEMISTRY
(2023)
Review
Chemistry, Multidisciplinary
Brendan L. Murphy, Francois P. Gabbai
Summary: This article introduces the research on the use of antimony compounds as new platforms for anion capture, sensing, and transport, emphasizing the excellent Lewis acidic properties of antimony and its potential in supramolecular chemistry and catalysis. It also mentions the recent advances in anion sensing in aqueous media and anion binding catalysis and anion transport across phospholipid membranes.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Inorganic & Nuclear
Asima Munawar, Logan T. Maltz, Wei-Chun Liu, Francois P. Gabbai
Summary: This study presents the design of a novel ligand structure, allowing facile introduction of cationic charge through methylation, to investigate the effect of positive charge insertion on the catalytic activity of gold catalysts. Experimental results demonstrate significant differences in catalytic activity between neutral and cationic gold species.
Article
Chemistry, Multidisciplinary
Alessio Cataldo, Matus Chvojka, Gyeongjin Park, Vladimir Sindelar, Francois P. Gabbai, Stephen J. Butler, Hennie Valkenier
Summary: Here we introduce a novel approach using a europium(iii) complex to monitor the transmembrane transport of fluoride into liposomes. By utilizing the long emission lifetime of this probe, we are able to accurately measure the transport activity of fluorescent transporters. The high sensitivity, selectivity, and versatility of this assay enable us to investigate various types of fluoride transporters and unravel their mechanisms of action.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Benyu Zhou, Shantabh Bedajna, Francois P. Gabbai
Summary: The design of a gold catalyst activation system through the formation of a pnictogen bond with a neighboring antimony unit is described. The resulting complex shows efficient catalytic reactivity, possibly through an intramolecular Au-Cl -> Sb(v) interaction for carbophilic catalysis.
CHEMICAL COMMUNICATIONS
(2023)
