Article
Chemistry, Physical
Jiahao Liu, Yinwu Li, Jingxing Jiang, Yan Liu, Zhuofeng Ke
Summary: The study systematically provided mechanistic scenarios including boryl-directed (BD) oxidative addition, nondirected (nonBD) oxidative addition, and boryl-metal cooperation via B-hydrido type (BHMC) or B-carbanion type (BCMC) mechanisms to elucidate the role of a Lewis acidic boryl group in selective o-C-H activation of pyridine with PBP-Ir complexes. The results suggest the plausibility of BD and BCMC mechanisms, while nonBD and BHMC mechanisms are less preferred due to weak interactions and large distortions. Various PBP-Ir complexes have been evaluated to further explore the guidelines of this mechanistic understanding for the rational design of Lewis acid-transition-metal catalysts.
Article
Chemistry, Physical
Olga B. Morozova, Alexandra V. Yurkovskaya
Summary: The second-order rate constants of histidine radicals reduced by tryptophan were obtained for different combinations of amino acids and their N-acetyl derivatives. Contributions from inter- and intramolecular reduction were revealed for the dipeptide N-acetyl histidine-tryptophan. The pH dependences of the rate constants were determined by the protonation state of tryptophan's amino group, suggesting a possible reaction mechanism of proton coupled electron transfer.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Biochemistry & Molecular Biology
Zhihao Niu, Qiaozhuo Wu, Qingzhong Li, Steve Scheiner
Summary: The tetrel bond between 1,2-benzisothiazol-3-one-2-TF3-1,1-dioxide (T = C, Si) and pyridine-1-oxide (PO) and its derivatives (PO-X, X = H, NO2, CN, F, CH3, OH, OCH3, NH2, and Li) was investigated using quantum chemical methods. The Si-O tetrel bond is strong, with interaction energies reaching a maximum of nearly 70 kcal/mol, while the C-O tetrel bond is weaker, with interaction energies between 2.0 and 2.6 kcal/mol. The presence of an electron-withdrawing substituent weakens the tetrel bond, while an electron-donating group strengthens it. The SiF3 group transfers approximately halfway between the acid's nitrogen and the base's oxygen without the assistance of cooperative effects from a third entity.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Chemistry, Applied
Jin Xu, Yuhao Zhang, Ke Du, Wei Yang
Summary: A benzo[b] naphtho[1,2-d]thiophene-S,S-dioxide (NSO) electron-deficient acceptor was synthesized to lower the electron-withdrawing ability. The copolymers PPF-NSs and PPF-NSOs were studied, and it was found that intermolecular energy transfer was the main mechanism of photoluminescence for PPF-NSs, while intramolecular charge transfer played the main role for PPF-NSOs. PPF-NSOs showed superior blue emission at a low acceptor concentration, while the energy transfer-based copolymer PPF-NS1 also achieved satisfactory performance.
Article
Chemistry, Organic
Ethan A. Gormong, Dorian S. Sneddon, Theresa M. Reineke, Thomas R. Hoye
Summary: The presence of a nearby tethered functional group significantly affects the cleavage rate of an Si-O bond. In this study, we investigated the relative rates of cleavage of model substrates with different Si-O substructures using in situ H-1 NMR spectroscopy. The computed trends in the relative rates correlated well with the experimental data. Additionally, we observed a siloxy-metathesis reaction facilitated by a pendant dimethylamino group.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Zhuangzhuang Ma, Xinzhen Ji, Meng Wang, Fei Zhang, Zibin Liu, Dongwen Yang, Mochen Jia, Xu Chen, Di Wu, Yu Zhang, Xinjian Li, Zhifeng Shi, Chongxin Shan
Summary: Perovskite light-emitting diodes (LEDs) are promising light sources for future lighting and display technologies. However, achieving yellow electroluminescence, environmental stability, and lead toxicity are challenges. By incorporating a hole-transporting polymer into the CsCu2I3 emitter, the electroluminescent performance of the LEDs is improved, resulting in significantly enhanced device performances. The external quantum efficiency of the yellow LEDs is increased by 8.5 times, and the half-lifetime reaches 14.6 hours, making them the most stable yellow LEDs based on perovskite systems reported so far.
Article
Chemistry, Inorganic & Nuclear
Shi-Nuo Xu, Yan Zheng, Jing-Yao Ye, Zhong-Yang Chen, Jian-Feng Yan, Yan-Hou Geng, Wenjing Hong, Yao-Feng Yuan
Summary: Here, we present the synthesis, structure, and single-molecule conductance of three o-carborane-based molecular wires with multiple conduction channels. Through experimental and theoretical studies, we found that o-carborane-based wires have a unique three-dimensional structure that facilitates through-space transmission paths and stable molecular junction formation compared to phenyl-centered wires. The significant difference in conductance is attributed to the combination of multiple conduction channels and quantum interference. Understanding the impact of different bridging groups and anchor group substitution patterns provides valuable insights for designing multichannel molecular wires based on o-carboranes.
DALTON TRANSACTIONS
(2023)
Article
Biochemistry & Molecular Biology
Cheng-Hsin Huang, Tong Wai Wong, Chen-Hsu Yu, Jing-Yuan Chang, Shing-Jong Huang, Shou-Ling Huang, Richard P. Cheng
Summary: This study demonstrates the importance of cross-strand lateral ion-pairing interactions for antiparallel beta-sheet stability, with the swapping of charged residues positions not significantly affecting interaction dynamics. Most swapped peptides showed higher folding populations, indicating the significance of lateral ion-pairing interactions in protein structures.
Article
Chemistry, Multidisciplinary
Renyou Yu, Yongjun Song, Ke Zhang, Xianchun Pang, Mingxing Tian, Lei He
Summary: This study demonstrates the development of efficient, bright, and stable LECs using intrinsically-ionic TADF materials 1-3, showcasing excellent performance characteristics.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Physical
Arthit Nueangaudom, Somsak Pianwanit, Haruhiko Tamaoki, Yasuzo Nishina, Fumio Tanaka, Seiji Taniguchi, Haik Chosrowjan
Summary: The molecular interactions between o-aminobenzoate (oAB) and isoallxazine (Iso) in the o-aminobenzoate D-amino acid oxidase complex (ODC) were studied using molecular dynamics simulation (MDS) and molecular orbital (MO) method. Results showed the formation of hydrogen bonds, charge transfer (CT) band, and fluorescence in the complex, indicating different states and interactions between oAB and Iso.
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
(2021)
Article
Biochemical Research Methods
Shivani Sharma, Joy Debnath, Kalyan Sundar Ghosh
Summary: Schiff base probes 1 and 2 were developed as highly selective fluorimetric chemosensors for Cu2+ and Al3+ ions respectively. The fluorescence emission of probe 1 at 415 nm was quenched by Cu2+, while the weak fluorescence of probe 2 at 506 nm was specifically enhanced by Al3+. The metal ion-probe complexation stoichiometry was found to be 1:1. The probes showed low detection limits of 9.9 and 2.5 nM for Cu2+ and Al3+ respectively. The sensing mechanisms were proposed based on density functional theory and spectroscopic results. Probe 1 was also used in a logic gate for Cu2+ detection, and both probes were applied for quantitative estimation of Cu2+ and Al3+ in water samples.
Article
Chemistry, Multidisciplinary
Zhennan Zhao, Cheng Zeng, Xiaomei Peng, Yuchao Liu, Haisong Zhao, Lei Hua, Shi-Jian Su, Shouke Yan, Zhongjie Ren
Summary: A series of ultrapure-blue thermally activated delayed fluorescence (TADF) emitters featuring through-space charge transfer (TSCT) have been constructed, which exhibit accelerated radiative transition, diminished vibrionic relaxation, reduced Stokes shift, and narrow emission. The corresponding OLEDs based on AC-BO and QAC-BO demonstrate excellent performance with EQE(max) of 19.3% and 15.8%, respectively.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Anirban Karmakar, Anup Paul, Ines R. M. Santos, Pedro M. R. Santos, Elia Pantanetti Sabatini, Atash V. Gurbanov, M. Fatima C. Guedes da Silva, Armando J. L. Pombeiro
Summary: In this study, four new zinc(II) coordination polymers (CPs) were synthesized and characterized. CP 1, with an anthracene group, showed the highest efficiency in removing various cationic and anionic dyes. CPs 3 and 4, tagged with pyrene, selectively removed cationic dyes.
CRYSTAL GROWTH & DESIGN
(2022)
Article
Chemistry, Physical
Shiho Yada, Miyako Wakizaka, Hiroshi Shimosegawa, Hiroya Fujita, Munehiro Yamada, Yukako Matsue, Tomokazu Yoshimura
Summary: The interfacial adsorption properties of a novel hydroxy-group-containing amino-acid-type surfactant and a conventional hydroxy-group-free amino-acid-type surfactant were investigated in an alkaline solution. The novel surfactant showed a lower critical micelle concentration and nonionic-like behavior due to hydrogen bonding between hydroxy groups and carboxylate ions, which reduced electrostatic repulsion between hydrophilic groups.
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
(2021)
Article
Chemistry, Multidisciplinary
Virginia Valderrey, Kornelia Gawlitza, Knut Rurack
Summary: Bifunctional fluorescent molecular oxoanion probes based on the benzoxadiazole (BD) chromophore are developed in this study. These probes integrate a thiourea binding motif and a polymerizable 2-aminoethyl methacrylate unit in the core, and exhibit strongly Stokes shifted absorption and fluorescence due to concerted charge transfer. By binding electron-rich carboxylate guests, the emission of the probes further red-shifts, allowing for detection of antibiotics in highly polar solvents.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)