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Synthesis, Structure, and Redox Reactivity of Ni Complexes Bearing a Redox and Acid-Base Non-innocent Ligand with Ni, Ni, and Ni Formal Oxidation States.
J Am Chem Soc
January 2025
Department of Chemistry and Nano Science, Ewha Womans University, Seoul 03760, Korea.
A series of Ni complexes bearing a redox and acid-base noninnocent tetraamido macrocyclic ligand, H-(TAML-4) {H-(TAML-4) = 15,15-dimethyl-5,8,13,17-tetrahydro-5,8,13,17-tetraaza-dibenzo[]cyclotridecene-6,7,14,16-tetraone}, with formal oxidation states of Ni, Ni, and Ni were synthesized and characterized structurally and spectroscopically. The X-ray crystallographic analysis of the Ni complexes revealed a square planar geometry, and the [Ni(TAML-4)] complex with the formal oxidation state of Ni was characterized to be [Ni(TAML-4)] with the oxidation state of the Ni ion and the one-electron oxidized TAML-4 ligand, TAML-4. The Ni oxidation state and the TAML-4 radical cation ligand, TAML-4, were supported by X-ray absorption spectroscopy and density functional theory calculations.
View Article and Find Full Text PDFProton-Controlled Electron Injection in MoS During Hydrogen Evolution Revealed by Time-Resolved Spectroelectrochemistry.
J Am Chem Soc
January 2025
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
Monolayer MoS is an effective electrocatalyst for the hydrogen evolution reaction (HER). Despite significant efforts to optimize the active sites, its catalytic performance still falls short of theoretical predictions. One key factor that has often been overlooked is the electron injection from the conductive substrate into the MoS.
View Article and Find Full Text PDFPreparation of novel lithiated high-entropy spinel-type oxyhalides and their electrochemical performance in Li-ion batteries.
Nanoscale
January 2025
J. Heyrovský Institute of Physical Chemistry, Czech Acad. Sci., Dolejškova 3, CZ-18200, Prague 8, Czech Republic.
Compositionally complex doping of spinel oxides toward high-entropy oxides is expected to enhance their electrochemical performance substantially. We successfully prepared high-entropy compounds, the oxide (ZnMgCoCu)FeO (HEOFe), lithiated oxyfluoride Li(ZnMgCoCu)FeOF (LiHEOFeF), and lithiated oxychloride Li(ZnMgCoCu)FeOCl (LiHEOFeCl) with a spinel-based cubic structure by ball milling and subsequent heat treatment. The products exhibit particles with sizes from 50 to 200 nm with a homogeneous atomic distribution.
View Article and Find Full Text PDFThe Influence of Alkyl Spacers and Molecular Weight on the Charge Transport and Storage Properties of Oxy-Bithiophene-Based Conjugated Polymers.
Angew Chem Int Ed Engl
December 2024
Department of Physics and Centre for Processable Electronics, Imperial College London, SW7 2AZ, London, United Kingdom.
Conjugated polymers (CPs) with polar side chains can conduct electronic and ionic charges simultaneously, making them promising for bioelectronics, electrocatalysis and energy storage. Recent work showed that adding alkyl spacers between CP backbones and polar side chains improved electronic charge carrier mobility, reduced swelling and enhanced stability, without compromising ion transport. However, how alkyl spacers impact polymer backbone conformation and, subsequently, electronic properties remain unclear.
View Article and Find Full Text PDFCyclo[4]pyrrole with - direct linkages.
Chem Sci
November 2024
Division of Applied Chemistry, Faculty of Engineering, Hokkaido University Kita 13, Nishi 8, Kita-ku Sapporo Hokkaido 060-8628 Japan
A cyclo[4]pyrrole bearing pyrrole C()-C() direct linkages, a contracted porphyrin analogue with no -carbon bridge, was synthesized from an oligoketone-related precursor. X-ray crystallography and StrainViz analysis revealed a non-planar structure with a total strain of 20.8 kcal mol.
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