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Exploring Singlet Carbyne Anions and Related Low-Valent Carbon Species Utilizing a Cyclic Phosphino Substituent.
Acc Chem Res
January 2025
Department of Chemistry and Research Center for Chemical Biology and Omics Analysis, College of Science, Southern University of Science and Technology, Shenzhen 518055, China.
ConspectusThe advancement of synthetic methodologies is fundamentally driven by a deeper understanding of the structure-reactivity relationships of reactive key intermediates. Carbyne anions are compounds featuring a monovalent anionic carbon possessing four nonbonding valence electrons, which were historically confined to theoretical constructs or observed solely within the environment of gas-phase studies. These species possess potential for applications across diverse domains of synthetic chemistry and ancillary fields.
View Article and Find Full Text PDFGuarding Drinking Water Safety against Harmful Algal Blooms: Could UV/Cl Treatment Be the Answer?
Environ Sci Technol
January 2025
Environmental Engineering and Science, Department of Chemical and Environmental Engineering (ChEE), University of Cincinnati, Cincinnati, Ohio 45221, United States.
Frequent and severe occurrences of harmful algal blooms increasingly threaten human health by the release of microcystins (MCs). Urgent attention is directed toward managing MCs, as evidenced by rising HAB-related do not drink/do not boil advisories due to unsafe MC levels in drinking water. UV/chlorine treatment, in which UV light is applied simultaneously with chlorine, showed early promise for effectively degrading MC-LR to values below the World Health Organization's guideline limits.
View Article and Find Full Text PDFComputational Study of SmI-Catalyzed Intermolecular Couplings of Cyclopropyl Ketones: Links between the Structure and Reactivity.
J Org Chem
November 2024
Department of Chemistry, School of Natural Sciences, The University of Manchester, ManchesterM13 9PL, U.K.
Article Synopsis
- SmI-catalyzed reactions involving cyclopropyl ketones and alkenes or alkynes can create diverse five-membered ring structures through systematic computational analysis.
- Aryl cyclopropyl ketones show enhanced reactivity due to stabilizing effects from the aryl ring, despite challenges from intermediate energy barriers, while alkyl cyclopropyl ketones face higher barriers but enable easier radical trapping.
- The study highlights that bicyclo[1.1.0]butyl ketones have increased reactivity due to their strained structure, whereas bicyclo[2.1.0]pentyl ketones, being less strained, demonstrate efficient coupling due to stable fragmentation intermediates.
Structure-Reactivity Relationships in a Small Library of Imine-Type Dynamic Covalent Materials: Determination of Rate and Equilibrium Constants Enables Model Prediction and Validation of a Unique Mechanical Softening in Dynamic Hydrogels.
J Am Chem Soc
October 2024
Department of Instructive Biomaterials Engineering, MERLN Institute for Technology-Inspired Regenerative Medicine, Maastricht University, 6229 ER Maastricht, The Netherlands.
The development of next generation soft and recyclable materials prominently features dynamic (reversible) chemistries such as host-guest, supramolecular, and dynamic covalent. Dynamic systems enable injectability, reprocessability, and time-dependent mechanical properties. These properties arise from the inherent relationship between the rate and equilibrium constants (RECs) of molecular junctions (cross-links) and the resulting macroscopic behavior of dynamic networks.
View Article and Find Full Text PDFExperimentally validating sabatier plot by molecular level microenvironment customization for oxygen electroreduction.
Nat Commun
July 2024
College of Chemistry and Chemical Engineering/Film Energy Chemistry for Jiangxi Provincial Key Laboratory (FEC), Nanchang University, Nanchang, 330031, PR China.
Microenvironmental modifications on metal sites are crucial to tune oxygen reduction catalytic behavior and decrypt intrinsic mechanism, whereas the stochastic properties of traditional pyrolyzed single-atom catalysts induce vague recognition on structure-reactivity relations. Herein, we report a theoretical descriptor relying on binding energies of oxygen adsorbates and directly associating the derived Sabatier volcano plot with calculated overpotential to forecast catalytic efficiency of cobalt porphyrin. This Sabatier volcano plot instructs that electron-withdrawing substituents mitigate the over-strong *OH intermediate adsorption by virtue of the decreased proportion of electrons in bonding orbital.
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