Article
Multidisciplinary Sciences
Francesca M. Ippoliti, Nathan J. Adamson, Laura G. Wonilowicz, Daniel J. Nasrallah, Evan R. Darzi, Joyann S. Donaldson, Neil K. Garg
Summary: Small rings containing allenes are unconventional compounds that have been known since the 1960s. Despite having similar discovery time to benzyne and advantageous features, strained cyclic allenes have been underutilized in chemical synthesis. This study presents a concise total synthesis of lissodendoric acid A, a manzamine alkaloid, through the selective trapping of a short-lived cyclic allene intermediate. This synthetic approach efficiently constructs the azadecalin framework, resulting in a 12-step total synthesis with a 0.8% overall yield.
Article
Chemistry, Multidisciplinary
Qianfeng Qiu, Sirun Yang, Mihael A. Gerkman, Heyifei Fu, Ivan Aprahamian, Grace G. D. Han
Summary: A new type of hydrazone photoswitch was developed, with a macrocyclic structure and phase transition feature, which can store a large amount of energy. It provides a promising strategy for molecular solar thermal energy storage applications.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Biochemistry & Molecular Biology
Alexander N. Grechkin, Natalia V. Lantsova, Lucia S. Mukhtarova, Bulat I. Khairutdinov, Svetlana S. Gorina, Tatiana M. Iljina, Yana Y. Toporkova
Summary: The product specificity and mechanistic peculiarities of two allene oxide synthases, namely tomato LeAOS3 and maize ZmAOS, were studied. Both enzymes were capable of producing 9,10-EOD and alpha-ketol, with ZmAOS mainly producing 9,10-EOD and LeAOS3 producing a mixture of 9(R)-alpha-ketol and 9,10-EOD. LeAOS3 also showed higher yields of cis-10-oxo-PEA and Favorskii-type product. These findings contribute to the understanding of the enzyme functionality and synthesis characteristics.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Chemistry, Multidisciplinary
Melissa Ramirez, Dennis Svatunek, Fang Liu, Neil K. Garg, Kendall N. Houk
Summary: The Diels-Alder reactions of furans and pyrroles with 1,2-cyclohexadiene and oxa- and azaheterocyclic analogs exhibit endo selectivity, which is determined by the interaction of molecular orbitals and electrostatic effects. This selectivity, based on stabilizing interactions, is expected to lead to the increased use of strained cyclic allenes in chemical synthesis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Physics, Applied
Inseo Kim, Hyungwoo Lee, Minseok Choi
Summary: In this study, the formation of oxygen vacancies in strained Ti-based oxides was investigated using first-principles density functional theory calculations and chemical bond analyses. The results showed clear correlations between structural features and strain, as well as similar trends for electronic features under different strains except for shear strains. The impact of strain on the formation of oxygen vacancies was also examined, revealing that the formation energy in strained oxides was linearly linked to changes in cell volume, bandgap, and Ti-O bond strength, except in compressively strained and shear-strained systems.
JOURNAL OF APPLIED PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Melissa Ramirez, Evan R. Darzi, Joyann S. Donaldson, Kendall N. Houk, Neil K. Garg
Summary: This study investigates the reaction of oxadiazinones and strained alkynes to produce PAHs through computational and experimental approaches. It was found that the use of different types of alkynes can lead to the synthesis of PAHs with varying symmetries, and experimental studies successfully produced new PAHs, including tetracene and pentacene.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Kota Koshino, Rei Kinjo
Summary: This study presents the synthesis of a dianionic dialane based on the Al2O three-membered ring scaffold, with a highly strained Al-Al sigma-bond. This compound can react with unsaturated substrates to form heterocycles, and selectively activate an arene ring C-C bond for further reactions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Dexia Zhou, Fang Zhang, Baihui Wang, Jiman He, Yimin Bai, Hongtao Bian
Summary: Anion recognition through noncovalent interactions is an emerging field in supramolecular chemistry. This study investigates the thermodynamics of complexation between sodium cyanate and calix[4]pyrrole, revealing enthalpy changes as the dominant driving force. Further analysis suggests that anion recognition in solution is mediated by conformational changes of the receptor and collective rearrangement of hydrogen bond dynamics.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Inorganic & Nuclear
Carlos Ferrer, Joaquina Ferrer, Vincenzo Passarelli, Fernando J. Lahoz, Pilar Garcia-Orduna, Daniel Carmona
Summary: This study reports the synthesis, characterization, and reactivity of dinuclear rhodium and iridium complexes based on N-pyridin-2-ylmethyl-N',N ''-bis-(2,6-diisopropylphenyl) guanidine (H2L) as a ligand. The complexes were found to activate the H-H and O-H bonds of dihydrogen and water, suggesting their potential application as catalysts or functional materials. The results provide important experimental evidence for exploring new catalysts and preparing functional materials.
Article
Chemistry, Multidisciplinary
Sushanth Kini Manjeshwar, Anastasiia Ciers, Fia Hellman, Juergen Blaesing, Andre Strittmatter, Witlef Wieczorek
Summary: Nanomechanical resonators made from tensile-strained materials have extremely low mechanical dissipation in the kHz to MHz frequency range. These materials also allow for the realization of monolithic free-space optomechanical devices with properties such as stability and scalability. In this study, we demonstrate nanomechanical string and trampoline resonators made from tensile-strained InGaP, and characterize their mechanical properties and performance.
Article
Chemistry, Inorganic & Nuclear
A. N. Vasiliev, P. S. Berdonosov, E. S. Kozlyakova, O. Maximova, A. F. Murtazoev, V. A. Dolgikh, K. A. Lyssenko, Z. Pchelkina, D. Gorbunov, S. H. Chung, H-J Koo, M-H Whangbo
Summary: Pb2Cu10O4(SeO3)(4)Cl-7 is a mixed-valence compound with a complex structure, consisting of nonmagnetic and magnetic copper ions. It exhibits antiferromagnetic ordering at low temperatures and a sequence of spin-flop transition and magnetization plateau formation. The magnetic properties of this compound can be described by the arrangement of copper clusters, and the 1/3 magnetization plateau is caused by the field-induced flip of the copper clusters within the unit cell.
DALTON TRANSACTIONS
(2022)
Article
Polymer Science
Rajeshwar Vasdev, Wilson Luo, Kyle Classen, Michael Anghel, Samantha Novoa, Mark S. Workentin, Joe B. Gilroy
Summary: This study demonstrates the use of cyclopropenone-masked strained alkynes to prepare functional polymers, opening the door to the creation of libraries of multifunctional chain-growth polymers with identical polymer backbones.
Article
Chemistry, Inorganic & Nuclear
Diana O. Nekrasova, Alexander A. Tsirlin, Marie Colmont, Oleg Siidra, Angel M. Arevalo-Lopez, Olivier Mentre
Summary: The study reveals that the lattice relaxation and insertion of neutral CuO species occur when replacing alkali metals with larger Rb and Cs ions. The magnetic properties show complex behavior of S = 1 Cu-14 spin clusters.
INORGANIC CHEMISTRY
(2021)
Article
Nanoscience & Nanotechnology
Wei Cao, Ziyu Wang, Ling Miao, Jing Shi, Rui Xiong
Summary: The high-temperature phase of Cu2Se, beta-Cu2Se, has attracted attention for its excellent thermoelectric efficiency. Studying the effect of strain and the possibility of n-type beta-Cu2Se is essential, with compressive strain promoting the power factor and tensile strain reducing lattice thermal conductivity. Predicted zT values for n-type and p-type beta-Cu2Se can reach 1.65 and 1.71 at 800 K respectively, and a feasible strategy to manipulate the lattice structure and carrier type is proposed through doping halogen elements.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Ulf R. Pedersen, Ian Douglass, Peter Harrowell
Summary: Through computer simulations, it has been established that the structure of a supercooled binary atomic liquid mixture consists of common neighbor structures similar to those found in the equilibrium crystal phase, a Laves structure. Despite the large accumulation of crystal-like structure, it is confirmed that the supercooled liquid represents a true metastable liquid and can borrow the crystal structure without being destabilized. The origin of all instances of liquids with a strongly favored local structure is being considered.
JOURNAL OF CHEMICAL PHYSICS
(2021)