Solid-state electrolytes are crucial for the realization of safe and high capacity all-solid-state batteries. Lithium-containing complex hydrides represent a promising class of solid-state electrolytes, but they exhibit low ionic conductivities at room temperature. Ion substitution and nanoconfinement are the main strategies to overcome this challenge. Here, we report on the synthesis of nanoconfined anion-substituted complex hydrides in which the two strategies are effectively combined to achieve a profound increase in the ionic conductivities at ambient temperature. We show that the nanoconfinement of anion substituted LiBH (LiBH-LiI and LiBH-LiNH) leads to an enhancement of the room temperature conductivity by a factor of 4 to 10 compared to nanoconfined LiBH and nonconfined LiBH-LiI and LiBH-LiNH, concomitant with a lowered activation energy of 0.44 eV for Li-ion transport. Our work demonstrates that a combination of partial ion substitution and nanoconfinement is an effective strategy to boost the ionic conductivity of complex hydrides. The strategy could be applicable to other classes of solid-state electrolytes.
Download full-text PDF |
Source |
---|---|
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7011749 | PMC |
http://dx.doi.org/10.1021/acs.jpcc.9b10607 | DOI Listing |
J Biol Chem
December 2024
Structural Biochemistry, Department of Chemistry, Bielefeld University, Universitätsstraße 25, 33615 Bielefeld, Germany. Electronic address:
Two-component flavin-dependent monooxygenases are of great interest as biocatalysts for the production of pharmaceuticals and other relevant molecules, as they catalyze chemically important reactions such as hydroxylation, epoxidation and halogenation. The monooxygenase components require a separate flavin reductase, which provides the necessary reduced flavin cofactor. The tryptophan halogenase Thal from Streptomyces albogriseolus is a well-characterized two-component flavin-dependent halogenase.
View Article and Find Full Text PDFChem Sci
December 2024
Department of Chemistry, University of York Heslington YO10 5DD UK
This work details how the unusual iridium tetrahydride [Ir(H)(IMes)(sulfoxide)]Na and trihydride [Ir(H)(IMes)(sulfoxide)] can be formed in a solvent dependent reaction of [IrCl(COD)(IMes)] with sulfoxide (dimethyl or methylphenyl), base, and H. In the case of dimethyl sulfoxide, the four hydride ligands of the tetrahydride are equivalent, and the IMes and sulfoxide ligands mutually . However, for phenyl methyl sulfoxide, this isomer of the tetrahydride forms alongside its counterpart where the remarkable symmetry breaking effect of the sulfoxide leads to it presenting four chemically distinct hydride ligands.
View Article and Find Full Text PDFDalton Trans
December 2024
Leibniz Institute for Catalysis, Albert-Einstein-Str. 29a, 18059 Rostock, Germany.
Starting from the alkyne complex CpZr(py)(η-MeSiCSiMe) (Cp = η-cyclopentadienyl, py = pyridine), the synthesis and complete characterisation of a zirconocene(IV) triazenido hydride complex and its use in the activation of small molecules is reported. The reaction with CO led to the formation of a zirconocene(IV) triazenido-formate complex, which was further investigated for its stability towards different bases with respect to the formation of formic acid. The experimentally observed reaction pathway was investigated computationally using DFT methods, revealing the favourable role of pyridine coordination in the hydrogen transfer from the triazene to the alkyne unit of the zirconocene reagent.
View Article and Find Full Text PDFDalton Trans
December 2024
Department of Chemistry, Graduate School of Science, Tohoku University, Sendai 980-8578, Japan.
Effective activation of small molecules (alcohol, phenol, ketones, amine, .) by a hydrogen-bridged bis(silylene) complex, which has two adjacent Lewis acidic centers and a hydridic bridging hydrogen with weak Si⋯H bonds, is described, along with product characterization by NMR and X-ray diffraction studies.
View Article and Find Full Text PDFInorg Chem
December 2024
Department of Chemistry, University of Toronto, 80 Saint George Street, Toronto, Ontario M5S-3H6, Canada.
Here it is demonstrated that there is a linear relationship between the terminal 3d metal hydride stretching wavenumber ν and the metal hydride distance reported to date: ν ∼ (-1.05 + 3.35) × 10 cm.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!