Article
Chemistry, Physical
Sara Yacob, Michael Caulfield, Robert B. Larson, Elaine Gomez, Randall J. Meyer
Summary: The importance of chemicals in a low carbon future highlights the need to reduce CO2 emissions associated with their production. Process conceptualization can help identify key catalytic variables that influence emissions while maintaining competitiveness. This approach was applied to ethylene production, comparing different routes and identifying key catalytic variables that can reduce emissions.
Article
Chemistry, Medicinal
Stephen Neidle
Summary: The role of G-quadruplexes in human cancers is well-defined and they can serve as potential drug targets. This study analyzed the role of bound water molecules in G-quadruplex-small molecule complexes, revealing the essential role of structured water molecules in mediating interactions between ligands and DNA.
Article
Chemistry, Physical
Zhijiang Jin, Hongchao Wang, Jie Shi, Hao Wang, Xiao Gao, Qian Gao, Xiaoli Sun
Summary: In this study, the role of indium and tin in Al-Ga based alloys was revealed through simulation and validation experiments. It was found that indium induces deeper and wider cracks inside the alloy, making it easier to break during hydrolysis and ensuring higher yields, while tin facilitates the reaction rate. A novel Al matrix embrittlement mechanism based on low-melting-point phases was proposed.
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Physical
Debotra Sarkar, Lisa Groll, Dominik Munz, Franziska Hanusch, Shigeyoshi Inoue
Summary: The aryl(imino)stannylene (Mes)Ter[N(IDipp)]Sn, stabilized by the NHI ligand, enables the sequestration and valorization of CO2 to C1 feedstock stoichiometrically, as well as catalytically. The NHI ligand plays a key role in the CO2 reduction process, rationalized by experimental and computational analysis.
Review
Biochemistry & Molecular Biology
Dongliang Hu, Lijuan Wei, Weibiao Liao
Summary: This review discusses the interaction between brassinosteroids (BRs) and small-molecule compounds (SMCs) in plant growth, development, and stress responses, highlighting how they promote plant development and alleviate stress damage by modulating the antioxidant system, photosynthetic capacity, and carbohydrate metabolism.
Article
Chemistry, Physical
Yan Chen, Jia-Jun Deng, Wen-Wen Yao, Joseph Israel Gurti, Wei Li, Wen-Jie Wang, Jian-Xi Yao, Xun-Lei Ding
Summary: Structures of non-stoichiometric MoxSy clusters were studied using density functional calculations, revealing a novel grid structure and the preference of hydrogen molecule adsorption onto Mo atoms. Additionally, vacant bridge sites between Mo-Mo in sulfur-deficient clusters were found to play a crucial role in hydrogen atom adsorption and transfer.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Review
Chemistry, Analytical
Haonan Li, Yuxi Fang, Junjie Yan, Xiangyu Ren, Chao Zheng, Bo Wu, Siyuan Wang, Zhanlin Li, Huiming Hua, Peng Wang, Dahong Li
Summary: Hydrogen sulfide (H2S) is considered as another gasotransmitter involved in important physiological and pathological processes. To real-time detect H2S in biological systems, numerous small-molecule fluorescent probes have been developed, with improvements in selectivity, response capability, and optical performance.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2021)
Review
Biochemistry & Molecular Biology
Lianne J. H. C. Jacobs, Jan Riemer
Summary: Compartmentalisation of eukaryotic cells enables the coexistence of different cellular processes. Small redox molecules, in cooperation with proteins, establish specific subcellular redox compartments that support oxidative protein folding and redox signaling. Dysregulated redox homeostasis is directly linked to various diseases. This review focuses on the mechanisms regulating redox homeostasis in the mitochondrial subcompartments of mammalian cells.
Article
Chemistry, Analytical
B. Zakhele Ndala, P. Ndivhuwo Shumbula, Siyabonga Nkabinde, Tshwarela Kolokoto, Siziwe Gqoba, Cebisa Linganiso, Nosipho Moloto
Summary: In this study, the catalytic performance of colloidal synthesized SnSe2 nanoplates towards the hydrogen evolution reaction (HER) was improved through electrochemical activation, resulting in exceptional catalytic activity.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Analytical
Fang Hu, Yunxia Huang, Yansheng Xiao, Yanchun Li, Xiao Luo, Xuhong Qian, Youjun Yang
Summary: By combining a Hill-type pH probe and a pH-insensitive naphthalimide fluorophore, a FRET-based ratiometric pH probe was synthesized with reduced pH transition width, providing a unique approach for detecting biorelevant pH changes efficiently.
ANALYTICAL METHODS
(2021)
Review
Chemistry, Multidisciplinary
Hai-Hao Han, He Tian, Yi Zang, Adam C. Sedgwick, Jia Li, Jonathan L. Sessler, Xiao-Peng He, Tony D. James
Summary: This tutorial review discusses the importance of chemical tools in real-time monitoring of organ function and visualization of organ-related processes at the cellular level in biological research. It highlights the potential of small-molecule fluorescent probes in advancing the understanding of organ-related diseases and emphasizes the need for probes with high sensitivity, low limit of detection, fast response times, and appropriate biocompatibility.
CHEMICAL SOCIETY REVIEWS
(2021)
Article
Chemistry, Multidisciplinary
Faisal Al-Odail, Javed Mazher
Summary: This study investigates the adsorption and dissociation of hydrogen molecules on small PdnAgm (n + m <= 4) clusters using density functional theory calculations. The results reveal that the cluster size and composition play a key role in determining the nature of the adsorption process. Molecular adsorption is more favorable on Pd atoms and mixed clusters, while hydrogen dissociation is more favorable on Pd-n (n = 2-4) clusters. The analysis of natural bond orbitals and density of states provides insights into the electron transfer between the hydrogen atoms and the metal clusters.
STRUCTURAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Aliona G. Baradzenka, Melanie Pilkington, Anton Dmitrienko, Georgii I. Nikonov
Summary: Reduction of (NP)PCl2 with KC8 yielded the phosphinoamidinato-supported phosphinidene (NP)P. Reaction of (NP)P with a N-heterocyclic carbene resulted in the NHC-adduct NHC?P-P(Pr-2(i))=NC(Ph)=NAr featuring an iminophosphinyl group. Various metathesis products were obtained through reactions of (NP)P with HBpin, H3SiPh, HPPh2, and tetrachlorobenzaquinone, including (NP)Bpin, (NP)SiH2Ph, and a base-stabilized phosphido-phosphinidene.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Mechanics
Yue Ma, Mingming Guo, Yi Zhang, Jialing Le, Ye Tian, Shuhong Tong, Hua Zhang, Fei Tang, Zeyang Zhao
Summary: This paper discusses in detail the generic inlet based on a smooth Bezier curve and the results and insights from high-dimensional dynamic multi-objective optimization. The optimization is achieved by integrating a Kriging surrogate model-assisted improved congestion distance multi-objective particle swarm optimization algorithm and computational fluid dynamics simulation. The results demonstrate a high total pressure recovery capability for the generic inlet, while meeting the requirements of surface area and drag. Additionally, grouping the obtained Pareto solution set using K-means feature recognition contributes to a comprehensive understanding of the flow physics knowledge related to optimal geometric local shape control.
Review
Biochemistry & Molecular Biology
Emma Danelius, Steve Halaby, Wilfred A. van der Donk, Tamir Gonen
Summary: The MicroED method allows high-resolution structural data to be collected from vanishingly small crystals, originally developed for studying proteins, it is also powerful for smaller systems like natural products, with promising impact on the field of small molecule research.
NATURAL PRODUCT REPORTS
(2021)
Article
Chemistry, Multidisciplinary
Alexa Caise, Agamemnon E. Crumpton, Petra Vasko, Jamie Hicks, Caitilin McManus, Nicholas H. Rees, Simon Aldridge
Summary: This study reports the synthesis of a distannyne supported by a pincer ligand with pendant amine donors, which can activate E-H bonds at tin centers through dissociation of N-Sn donor/acceptor interactions. This chemistry allows the assembly of mixed-valence tin atom chains, with a decreasing propensity for chain growth as chain length increases, potentially due to the electron-withdrawing properties of the -Sn(Ar)H- backbone units generated via oxidative addition.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Joschua Helmer, Olli J. Pakkanen, Chris Gendy, Alexander Hepp, Heikki M. Tuononen, Felicitas Lips
Summary: This study reveals a unique reaction cascade mechanism to synthesize a new silaheterocycle through reductive debromination, involving unprecedented two-fold intramolecular cycloaddition by transient silylenes. The key intermediates in the reaction mechanism were identified through experimental and computational analyses.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Kristian L. Mears, Cary R. Stennett, James C. Fettinger, Petra Vasko, Philip P. Power
Summary: A series of alkali metal 1-adamantoxide complexes were synthesized, and it was found that only one out of three HOAd(1) molecules was reduced. X-ray diffraction study of the sodium derivative revealed the structure with two unreduced HOAd(1) donors and one reduced alkoxide. This is the first example of alkali metal reduction of an alcohol inhibited by London dispersion effects.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Li Feng Lim, Martyna Judd, Petra Vasko, Michael G. Gardiner, Dimitrios A. Pantazis, Nicholas Cox, Jamie Hicks
Summary: An isostructural series of heavy Group 14 E(I) radical anions (Ge, Sn, Pb), stabilized by a bulky xanthene-based diamido ligand, were synthesized and characterized. The E(II) precursor complexes were one-electron reduced with sodium naphthalenide in THF, yielding the charge-separated radical anions as sodium salts. The comprehensive characterization using EPR spectroscopy, X-ray crystallography, and DFT analysis revealed that the spin density of the unpaired electron is mainly located in a p-orbital of pi symmetry on the Group 14 center in all cases.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Inorganic & Nuclear
Feda'a M. Al-Qaisi, Abdussalam K. Qaroush, Ibrahim K. Okashah, Ala'a F. Eftaiha, Petra Vasko, Fatima Alsoubani, Timo Repo
Summary: By following green chemistry principles, a zinc curcumin complex was synthesized and used as a sustainable catalyst for the synthesis of cyclic carbonate from CO2 and epoxides. The complex exhibited outstanding catalytic activity and showed potential for the synthesis of renewable carbonates.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Jacob S. McMullen, Ryan Huo, Petra Vasko, Alison J. Edwards, Jamie Hicks
Summary: The synthesis, characterisation and reactivity of two isostructural anionic magnesium and calcium complexes are reported. The anionic hydrides exist as dimers held together by interactions between the two anions and bridging potassium cations. The hydrides are terminal and stabilized by interactions with the potassium cations. They can insert and couple CO under mild conditions to give the corresponding group 2 cis-ethenediolate complexes. These complexes can undergo salt elimination reactions with silyl chlorides, leading to small unsaturated disilyl ethers with a high percentage of their mass originating from CO.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Andreas Heilmann, Petra Vasko, Jamie Hicks, Jose M. Goicoechea, Simon Aldridge
Summary: The reactions of a terminal aluminium imide with oxygen-containing substrates were investigated as a means of using it as a main group transfer agent for the [NR](2-) fragment. Various transfers were demonstrated, including imide moiety transfer to [N-2], [CO], and [Ph(H)C] units. Mechanistic studies revealed intermediate complexes formed during the reactions, and the role of CO2 in releasing the imine compound.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Etienne A. LaPierre, Lara K. Watanabe, Brian O. Patrick, Jeremy M. Rawson, Heikki M. Tuononen, Ian Manners
Summary: In this study, the synthesis and properties of an acyclic carbene-stabilized diphospha(aminyl) PNP radical compound were reported. The radical compound exhibited a conjugated framework and showed facile one-electron oxidation and reduction to form nonclassical nitrenium and amide species. Additionally, the conformational flexibility of a cationic compound and the coordination chemistry of a formal amide were also explored.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Ross A. A. Jackson, Aidan J. R. Matthews, Petra Vasko, Mary F. F. Mahon, Jamie Hicks, David J. J. Liptrot
Summary: The potassium aluminyl complex K-2[Al{N(Dipp)SiMe3}(2)](2) was synthesized, representing the first example of an aluminyl anion supported by an acyclic ligand framework. Attempts to form the same structure with a larger ligand framework resulted in C-H cleavage. K-2[Al{N(Dipp)SiMe3}(2)](2) behaved as a nucleophilic source of aluminum, forming a monomeric, acyclic magnesium aluminyl complex when reacted with an electrophilic b-diketiminate supported magnesium(II) iodide.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Hannu T. Vuori, J. Mikko Rautiainen, Erkki T. Kolehmainen, Heikki M. Tuononen
Summary: This paper reports high-level computational data for 116 compounds of boron and compares them with experimental and computational benchmark values. Important trends and outliers are identified, and recommendations are made to revise some key quantities. The uncertainties associated with experimental values are found to exceed those of high-level calculations, prompting the need for a reevaluation of computational contributions. The applicability of the established group contribution values is demonstrated by comparing the results with existing experimental and computational values for large organoboron compounds.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Inorganic & Nuclear
Anna C. Booth, Petra Vasko, M. Angeles Fuentes, Bart Cornelissen, Stephen Faulkner, Simon Aldridge
Summary: 1,8-Bis(boronic ester) derivatives of naphthalene, as receptors for fluoride ions through B-F-B chelation, are difficult to synthesize. However, unsymmetrical complexes with a bridging B-F-B motif have been successfully synthesized and shown to effectively uptake F- ions.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Multidisciplinary
Kristian L. Mears, Michelle A. Kutzleb, Cary R. Stennett, James C. Fettinger, Derrick C. Kaseman, Ping Yu, Petra Vasko, Philip P. Power
Summary: The fragmentation reactions of complex [B(beta-pinane)(3)] and its analogues were studied. It was found that the stereochemistry of the terpene greatly affects the London dispersion interactions.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Inorganic & Nuclear
Petra Vasko, Cheuk W. Lau
Summary: In this study, a series of neutral compounds were studied computationally to predict their reactivity towards ammonia based on structural and electronic parameters. The differences in oxidative addition and coordination complex formation were investigated depending on the identity of the central element, and different evaluation methods were used for Werner complexes.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Multidisciplinary
Rui Zhang, Aleksi Eronen, Petra Vasko, Xiangze Du, Joseph Install, Timo Repo
Summary: A highly efficient conversion of xylose and acetylacetone to a new type of bisfuranic monomer was reported, with the reaction selectivity tunable by additives. This strategy shows remarkable carbon efficiency and has the potential to lead to innovations in bio-based polymer synthesis.
Article
Chemistry, Multidisciplinary
Braulio M. Puerta Lombardi, Ethan R. Pezoulas, Roope A. Suvinen, Alexander Harrison, Zachary S. Dubrawski, Benjamin S. Gelfand, Heikki M. Tuononen, Roland Roesler
Summary: Isomeric bis(aldiminium) salts with a 1,4-cyclohexylene framework were synthesized and their ditopic ligand competency was proven. The cis-isomer was shown to form an electron-rich olefin through a proton-catalyzed pathway, with a thermodynamically favorable C=C bond formation and a small activation barrier. Compounds that can be described as insertion products of the cis-isomer into E-H bonds of NH3, CH3CN, and H2O were also identified.
CHEMICAL COMMUNICATIONS
(2022)
