Lewis acid-base adducts between potassium dihydrogenpnictogenides [K(18c6)PnH] (Pn=P, As) and Trialkylgallanes (GaMe, GaEt, GatBu) as well as BH were synthesized. In the course of these investigations, we were able to fully characterize a row of compounds of the type [K(18c6)(thf)][PnH(ER)] (E=B: R=H; E=Ga: R=Me, Et, tBu). Based on the successful syntheses of these species, we also synthesized several compounds of the composition [K(18c6)(thf)][Pn(SiMe)(ER)] (n=1, 2) starting from [KPn(SiMe)] (Pn=P and As) and ER (E=B, Al, In: R=Me; E=Ga: R=Me, Et, tBu). All isolated compounds, were examined by NMR spectroscopy, infra-red spectroscopy and elemental analysis. A selection of the compounds presented were also examined by means of X-ray structure analysis on the single crystal. The obtained adducts of negatively charged [PnH] and [Pn(SiMe)] fragments with Lewis acids are a class of compounds that has scarcely been investigated to date.
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http://dx.doi.org/10.1002/chem.202404199 | DOI Listing |
J Am Chem Soc
January 2025
Center for Nanomedicine, Institute for Basic Science (IBS), Seoul 03722, Republic of Korea.
Perpendicular nanochannel creation of two-dimensional (2D) nanostructures requires highly controlled anisotropic drilling processes of the entire structure via void formation. However, chemical approaches for the creation of porosity and defects of 2D nanostructures have been challenging due to the strong basal plane chemical stability and the use of harsh reactants, tending to give randomly corroded 2D structures. In this study, we introduce Lewis acid-base conjugates (LABCs) as molecular drillers with attenuated chemical reactivity which results in the well-defined perpendicular nanochannel formation of 2D TiS nanoplates.
View Article and Find Full Text PDFNat Commun
January 2025
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, 130012, Changchun, P. R. China.
High-entropy metal-organic frameworks (HE-MOFs) hold promise as versatile materials, yet current rare examples are confined to low-valence elements in the fourth period, constraining their design and optimization for diverse applications. Here, a novel high-entropy, defect-rich and small-sized (32 nm) UiO-66 (ZrHfCeSnTi HE-UiO-66) has been synthesized for the first time, leveraging increased configurational entropy to achieve high tolerance to doping with diverse metal ions. The lattice distortion of HE-UiO-66 induces high exposure of metal nodes to create coordination unsaturated metal sites with a concentration of 322.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemistry and Chemical Biology, Rutgers, The State University of New Jersey, 123 Bevier Road, Piscataway, New Jersey 08854, United States.
Electrostatic interactions, hydrogen bonding, and solvation effects can alter the free energies of ionizable functional groups in proteins and other nanoporous architectures, allowing such structures to tune acid-base chemistry to support specific functions. Herein, we expand on this theme to examine how metal sites ( = H, Zn, Co, Co) affect the p of benzoic acid guests bound in discrete porphyrin nanoprisms () in CDCN. These host-guest systems were chosen to model how porous metalloporphyrin electrocatalysts might influence H transfer processes that are needed to support important electrochemical reactions (e.
View Article and Find Full Text PDFJ Colloid Interface Sci
December 2024
School of Chemical Engineering, The University of Adelaide, North Terrace, Adelaide, SA 5005, Australia. Electronic address:
Photocatalytic oxygen evolution reaction (OER) is pivotal for sustainable energy systems yet lacks high-performance catalysts capable of strong visible light absorption, robust charge dynamics, fast reaction kinetics, and high oxidation capability. Herein, we report the multiscale optimization of carbon nitride through the construction of porous curled carbon nitride nanosheets (CNA-B30) incorporating boron center/cyano group Lewis acid-base pairs (LABPs). The unique chemical and structural features of CNA-B30 extended the photoabsorption edges of π → π* and n → π* electronic transitions to 470 nm and 715 nm, respectively.
View Article and Find Full Text PDFSmall
December 2024
Academy of Scientific and Innovative Research (AcSIR), Ghaziabad, 201002, India.
A mixed-ligand-based thermo-chemically robust and undulated metal-organic framework (MOF) is developed that embraces carboxamide moiety-grafted porous channels and activation-induced generation of open-metal site (OMS). The guest-free MOF acts as an outstanding heterogeneous catalyst in Hantzsch condensation for electronically assorted substrates with low catalyst loading and short duration under greener conditions than the reported materials. Besides Lewis acidic OMS, the carboxamide group activates the substrate via two-point hydrogen bonding, highlighting the effectiveness of custom-made functionalities in this multi-component reaction.
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