Two new mononuclear Ru complexes Ru(bipa)(pic) (1; Hbipa = 6-(1H-benzo[d]imidazol-2-yl)picolinic acid, pic = 4-picoline) and Ru(pbic)(pic) (2; Hpbic = 2-(pyridin-2-yl)-1H-benzo[d]imidazole-7-carboxylic acid, pic = 4-picoline) based on anionic ligands were successfully synthesized, and characterized using NMR spectroscopy, mass spectrometry, and X-ray crystallography. These catalysts showed high activities and stabilities in water oxidation in homogeneous systems with a high turnover number of 2100 and a turnover frequency of 0.21 s for complex 1. The O-O band formation mechanism involved water nucleophilic attack. An active catalytic intermediate, i.e., Ru-OH, was detected using high-resolution mass spectrometry.
Download full-text PDF |
Source |
|---|---|
| http://dx.doi.org/10.1039/c6dt02056a | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Evaluation of the Arrhenius behavior of -dodecane radical cation (RH˙) reactivity with lanthanide ion-complexed ,,','-tetraoctyl diglycolamide (TODGA).
Phys Chem Chem Phys
January 2025
Department of Chemistry and Biochemistry, California State University at Long Beach, 1250 N. Bellflower Blvd., Long Beach, CA, 90840, USA.
Temperature-dependent rate constants for the reaction of the -dodecane radical cation (RH˙) with trivalent lanthanide ion-complexed ,,','-tetraoctyl diglycolamide (TODGA) over the range 10-40 °C have been determined using electron pulse radiolysis/transient absorption spectroscopy techniques. For the free ligand, an activation energy of = 20.4 ± 0.
View Article and Find Full Text PDFOn the gold(I)-catalyzed enantioselective addition of indole to diphenylallene via anion-binding catalysis.
Tetrahedron Lett
October 2024
Department of Chemistry, University of California, Berkeley, CA 94720, USA.
Neutral dual hydrogen bond donors (HBDs) are effective catalysts that enhance the electrophilicity of substrates or the Lewis/Brønsted acidity of reagents through an anion-binding mechanism. Despite their success in various enantioselective organocatalytic reactions, their application to transition metal catalysis remains rare. Herein, we report the activation of gold(I) precatalysts by chiral ureas, leading to enantioselective hydroarylation of allenes with indoles.
View Article and Find Full Text PDFMetal-Ligand Spin-Lock Strategy for Inhibiting Anion Dimerization in Li-Rich Cathode Materials.
J Am Chem Soc
January 2025
Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, School of Materials Science and Engineering, Peking University, Beijing 100871, P. R. China.
Anion dimerization poses a significant challenge for the application of Li-rich cathode materials (LCMs) in high-energy-density Li-ion batteries because of its deleterious effects, including rapid capacity and voltage decay, sluggish reaction kinetics, and large voltage hysteresis. Herein, we propose a metal-ligand spin-lock strategy to inhibit anion dimerization, which involves introducing an Fe-Ni couple having antiferromagnetic superexchange interaction into the LCM to lock the spin orientations of the unpaired electrons in the anions in the same direction. As proof of concept, we applied this strategy to intralayer disordered LiTiS (ID-LTS) to inhibit S-S dimerization.
View Article and Find Full Text PDFIdentifying and tuning coordinated water molecules for efficient electrocatalytic water oxidation.
Nat Commun
December 2024
Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xi'an, Shaanxi, China.
Coordination complexes are promising candidates for powerful electrocatalytic oxygen evolution reaction but challenges remain in favoring the kinetics behaviors through local coordination regulation. Herein, by refining the synergy of carboxylate anions and multiconjugated benzimidazole ligands, we tailor a series of well-defined and stable coordination complexes with three-dimensional supramolecular/coordinated structures. The coordinated water as potential open coordination sites can directly become intermediates, while the metal center easily achieves re-coordination with water molecules in the pores to resist lattice oxygen dissolution.
View Article and Find Full Text PDFProton Transfer Anionic Polymerization of Methyl Methacrylate with Ligands for Dual Control of Molecular Weight and Tacticity.
Precis Chem
December 2024
Department of Molecular and Macromolecular Chemistry, Graduate School of Engineering, Nagoya University, Furo-cho, Chikusa-ku, Nagoya 464-8603, Japan.
Dual control of the molecular weight and tacticity in proton transfer anionic polymerization (PTAP) of methyl methacrylate (MMA) was investigated by using various ligands in the presence of a bulky potassium base catalyst and an organic compound with a weakly acidic C-H bond as dormant species in toluene at 0 °C. The tacticity of the resulting poly(MMA) (PMMA) produced without ligands was nearly atactic (// = 22/54/24). However, the use of 18-crown-6 as a ligand afforded predominantly syndiotactic PMMA ( ≈ 58%), whereas the use of chiral bis(oxazoline) ligands gave slightly isotactic-rich PMMA ( ≈ 32%).
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!