The utilization of compounds from natural sources to prepare functional materials is of great importance. Herein, we describe for the first time the preparation of organic-inorganic hybrid catalysts by using natural phytic acid as building block. Zirconium phosphonate (Zr-PhyA) was synthesized by reaction of phytic acid and ZrCl4 and was obtained as a mesoporous material with pore sizes centered around 8.5 nm. Zr-PhyA was used to catalyze the mild and selective Meerwein-Ponndorf-Verley (MPV) reduction of various carbonyl compounds, e.g., of levulinic acid and its esters into γ-valerolactone. Further studies indicated that both Zr and phosphate groups contribute significantly to the excellent performance of Zr-PhyA.
ARTICLEThis journal is Catalytic transfer hydrogenation (CTH) of ethyl levulinate (EL) to γ-valerolactone (GVL) is a very attractive reaction in the field of biomass transformation. In this work, a new porous Zrcontaining catalyst with phenate group in its structure was prepared by the coprecipitation of 4hydroxybenzoic acid dipotassium salt and ZrOCl 2 (Zr-HBA) in water and characterized by powder X-Ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), N 2 adsorption-desorption, and Fourier transform infrared spectroscopy. The Zr-HBA was used as the catalyst for CTH of EL to GVL in the presence of isopropanol, and the effects of temperature, time, and amount of the catalyst on the reaction were studied. It was found that Zr-HBA was very active for the reaction and a GVL yield of 94.4% could be achieved. Meanwhile, the Zr-HBA could be reused at least five times without notable decrease in activity and selectivity. The main reason for the high catalytic activity of the Zr-HBA was that the existence of phenate in the structure of Zr-HBA increased the basicity of the catalyst, which is favourable to the CTH of EL.
Ionic liquid 1-benzyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([BnMIm][NTf2]) can promote the generation of the ˙OOH free radical and thereby efficiently transformed the β-O-4 lignin model compound 2-phenoxyacetophenone into benzoic acid and phenol using O2 as the oxidant. Furthermore, the IL-based metal-free catalytic system can also depolymerize other lignin model compounds and organosolv lignin effectively.
Poly(ethylene oxide) has been widely investigated as
a potential
separator for solid-state lithium metal batteries. However, its applications
were significantly restricted by low ionic conductivity and a narrow
electrochemical stability window (<4.0 V vs Li/Li+)
at room temperature. Herein, a novel molecular self-assembled ether-based
polyrotaxane electrolyte was designed using different functional units
and prepared by threading cyclic 18-crown ether-6 (18C6) to linear
poly(ethylene glycol) (PEG) via intermolecular hydrogen bond and terminating
with hexamethylene diisocyanate trimer (HDIt), which was strongly
confirmed by local structure-sensitive solid/liquid-state nuclear
magnetic resonance (NMR) techniques. The designed electrolyte has
shown an obviously increased room-temperature ionic conductivity of
3.48 × 10–4 S cm–1 compared
to 1.12 × 10–5 S cm–1 without
assembling polyrotaxane functional units, contributing to the enhanced
cycling stability of batteries with both LiFePO4 and LiNi0.8Co0.15Al0.05O2 cathode
materials. This advanced molecular self-assembled strategy provides
a new paradigm in designing solid polymer electrolytes with demanded
performance for lithium metal batteries.
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