Article
Chemistry, Multidisciplinary
Kyle A. Mason, Adam C. Pearcy, Zachary A. Christensen, Isaac K. Attah, Michael Meot-Ner (mautner), M. Samy El-Shall
Summary: The stepwise hydration of the benzonitrile radical cation with water molecules has been investigated, revealing the formation of a new class of clusters.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Qing Wen, Hao Fu, Zhen-yu Wang, Ying-de Huang, Zhen-jiang He, Cheng Yan, Jing Mao, Kehua Dai, Xia-hui Zhang, Jun-chao Zheng
Summary: This study proposes a strategy of interfacial engineering and in situ etching to address the challenges of zinc dendrites and side reactions in aqueous rechargeable zinc ion batteries. By introducing a zinc l-cysteine functional layer, the hydrophobicity of the zinc anode is improved, corrosion is mitigated, and uniform zinc deposition is guided. In addition, in situ etching of the zinc foil increases the electrochemical surface area and reduces interfacial resistance. The experimental results show that the Cys-Zn-coated zinc anode exhibits excellent cycling and rate performance.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Organic
Kenji Ota, Kazunori Nagao, Hirohisa Ohmiya
Summary: This method synthesizes sterically hindered alpha-hydroxy carbonyl compounds through radical-radical coupling. It allows for the use of primary, secondary, and tertiary aliphatic carboxylic acids to introduce various alkyl substituents onto ketone moieties of alpha-ketocarbonyls under mild reaction conditions.
Article
Chemistry, Physical
Jason J. Sorensen, Erick Tieu, Michael D. Morse
Summary: Resonant two-photon ionization spectroscopy was used to observe sharp predissociation thresholds in lanthanide sulfides and selenides, showing that these thresholds coincide with true 0 K bond dissociation energies. Measurements of the 0 K gaseous heat of formation for each molecule, ionization energies, and bond dissociation energies were reported. Trends in bonding for the lanthanide sulfides and selenides were discussed, with transition metal sulfides found to be 15.6% more strongly bound than corresponding selenides.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Olivia L. Garry, Michael Heilmann, Jingjia Chen, Yufan Liang, Xiaheng Zhang, Xiaoshen Ma, Charles S. Yeung, David Jonathan Bennett, David W. C. MacMillan
Summary: Replacing aryl rings with saturated carbocyclic structures is of great interest in drug discovery for improved pharmacokinetic properties. However, the synthesis of 2-substituted BCPs remains challenging and nonmodular. This study presents a generalizable strategy for bridge functionalization and demonstrates a streamlined pathway to diverse 2-substituted BCPs through radical C-H abstraction and metallaphotoredox protocols.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Li Zhang, Jiyao Yan, Dilgam Ahmadli, Zikuan Wang, Tobias Ritter
Summary: Direct C-H fluorination is an efficient strategy to construct aromatic C-F bonds, but the presence of other functional groups and the high energy barrier of C-F bond formation make the transformation challenging. In this study, a new concept for C-H nucleophilic fluorination without the formation of azaarene Meisenheimer intermediates was reported, achieving successful nucleophilic oxidative fluorination of quinolines through an asynchronous concerted F--e(-)-H+ transfer.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Shree S. Sowndarya, Peter C. St John, Robert S. Paton
Summary: The study shows that the long-term stability of organic radicals requires both thermodynamic and kinetic stability, and the molecular descriptors obtained through quantum chemical calculations can help predict the location of long-lived radicals. The radical stability score is an effective metric for evaluating stable radicals, outperforming thermodynamic scales based on bond dissociation enthalpies.
Article
Chemistry, Multidisciplinary
Jing Xiang, Min Peng, Yi Pan, Li-Juan Luo, Shun-Cheung Cheng, Xin-Xin Jin, Shek-Man Yiu, Wai-Lun Man, Chi-Chiu Ko, Kai-Chung Lau, Tai-Chu Lau
Summary: The study presented the first example of N-dealkylation of various alkylamines by a luminescent osmium(VI) nitrido complex induced by visible light.
Article
Chemistry, Physical
Jakob Heller, Ethan M. Cunningham, Jessica C. Hartmann, Christian van der Linde, Milan Oncak, Martin K. Beyer
Summary: In this study, infrared multiple photon dissociation spectroscopy was used to investigate the hydrated vanadium cation. The results revealed the fragmentation channels and spectral patterns of the cation at different cluster sizes, providing insights into the structural and chemical changes of the hydrated vanadium cation.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Inorganic & Nuclear
Matthieu Regnacq, Denis Lesage, Marte S. M. Holmsen, Karinne Miqueu, Didier Bourissou, Yves Gimbert
Summary: The study demonstrates the remarkable catalytic ability of (P,C)-cyclometalated Au(iii) complexes in the intermolecular hydroarylation of alkynes. The previous evidence of an outer-sphere mechanism is confirmed through the analysis of experimental data and DFT calculations. The evaluation of critical energies of dissociation of Au(iii) complexes with different substrates using energy-resolved mass spectrometry experiments and kinetic modeling supports the collisional model and its application to particularly fragile adducts.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Matthieu Regnacq, Denis Lesage, Marte S. M. Holmsen, Karinne Miqueu, Didier Bourissou, Yves Gimbert
Summary: In this study, the mechanism of (P,C)-cyclometalated Au(iii) complexes catalyzing the intermolecular hydroarylation of alkynes is confirmed through experimental data and theoretical calculations, as well as energy-resolved mass spectrometry experiments and kinetic modeling. The results support the previously proposed collisional model and provide insights into the application of this model on fragile adducts.
DALTON TRANSACTIONS
(2023)
Article
Physics, Atomic, Molecular & Chemical
Fan Yang, Rebecca Coates, Georgia C. Boles, P. B. Armentrout
Summary: Experimental hydration energies of Mn2+(H2O)(x) complexes (x=4-9) were determined using threshold collision-induced dissociation (TCID) with Xe. The results were compared with theoretical values, showing reasonable agreement.
INTERNATIONAL JOURNAL OF MASS SPECTROMETRY
(2021)
Article
Chemistry, Physical
Jakob Heller, Ethan M. Cunningham, Christian van der Linde, Milan Oncak, Martin K. Beyer
Summary: Controlled activation of water molecules is crucial for efficient water splitting, as shown by studying the insertion reaction of hydrated singly charged manganese ions using IRMPD and mass spectrometry techniques. Comparison of IRMPD spectra and quantum chemical calculations reveal that the inserted structure requires stabilization through hydration.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Alex A. Fertig, William W. Brennessel, James R. McKone, Ellen M. Matson
Summary: This study investigates the role of proton and electron transfer in facilitating small-molecule oxygen activation using an organofunctionalized vanadium oxide assembly. Results show that the reduced polyoxovanadate can mediate the concerted transfer of hydrogen atoms and electrons, providing insights into the reaction mechanism.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Alba Vargas-Caamal, Eugenia Dzib, Filiberto Ortiz-Chi, Albeiro Restrepo, Gabriel Merino
Summary: In this study, the interactions between hydrogen halide molecules and water moieties were analyzed. The stable HF and HCl aggregates do not undergo dissociation, while HBr and HI clusters do experience dissociation. The lowest energy structure of (HI)3(H2O)3 is a separated ion pair, but the structure with a bihalide anion is only slightly higher in energy. Various contact modes, including hydrogen bonds, halogen bonds, ionic and long-range contacts, were observed among the more stable structures.