The selective autoxidation for the synthesis of valuable oxygenates has provoked keen interest from both academic and industrial sectors. Although the generation of reactive oxygen species via oxygen attack on C-H bonds near ester linkages is well-established, research into aliphatic ester oxidation has primarily focused on combustion, neglecting their potential utility in oxidation processes. Herein, we demonstrated a protocol for producing propylene oxide through the autoxidation of ethyl acetate in tandem with propylene epoxidation.
View Article and Find Full Text PDFThe utilization of ferroelectric polarization-assisted photoelectrochemical (PEC) systems holds huge promise for solving the issue of high recombination of photogenerated electron-hole pairs. Monitoring their intricate charge-transfer process can offer profound insights into the advancement of highly active photoelectrodes. In this work, the hydrothermally synthesized titanium dioxide nanorod arrays (TiO NRAs) are subjected to etching to introduce oxygen vacancies (Ov), and subsequently loaded with barium titanate (BaTiO, BTO) nanoparticles to form a ferroelectric polarization effect-assisted type-II heterojunction.
View Article and Find Full Text PDFHerein, a high selective epoxidation of isobutene was achieved by heterogeneously dispersed MoSe with tert-butyl hydroperoxide (TBHP), which further showed versatile substrate scopes and well-retained activity among recycling tests. A rational mechanism is proposed based on extensive control experiments and electron paramagnetic resonance spectroscopy, surprisingly unveiling the metal-oxo and radical mediated pathways dramatically accelerated by hydrogen bonds of hexafluoroisopropanol (HFIP).
View Article and Find Full Text PDFBiVO is a promising photoanode for photoelectrochemical (PEC) water splitting but suffers from high charge carrier recombination and sluggish surface water oxidation kinetics that limit its efficiency. In this work, a model of sulfur-incorporated FeOOH cocatalyst-loaded BiVO was constructed. The composite photoanode (BiVO/S-FeOOH) demonstrates an enhanced photocurrent density of 3.
View Article and Find Full Text PDFDeveloping highly efficient catalytic protocols for C-sp(3)-H bond aerobic oxidation under mild conditions is a long-desired goal of chemists. Inspired by nature, a biomimetic approach for the aerobic oxidation of C-sp(3)-H by galactose oxidase model compound CuL and NHPI (-hydroxyphthalimide) was developed. The CuL-NHPI system exhibited excellent performance in the oxidation of C-sp(3)-H bonds to ketones, especially for light alkanes.
View Article and Find Full Text PDFUnder the background of carbon dioxide emission reduction, how to realize the treatment and the high value-added conversion of typical olefin volatile organic compounds (olefin-VOCs), such as styrene, is a big challenge. In this contribution, the ceria-supported coinage metal catalysts (M/CeO, M = Au, Ag, and Cu) are successfully synthesized by a dry mechanochemical method, and their catalytic performance for styrene-VOC epoxidation with tert-butyl hydrogen peroxide (TBHP) as an oxidant to prepare high-value styrene oxide (SO) is investigated. The oxygen vacancies of ceria play a key role in the anchoring of metal nanoparticles.
View Article and Find Full Text PDFPhotoelectrochemical (PEC) water splitting technology is a promising strategy toward producing sustainable hydrogen fuel. However, it is an essential bottleneck to reduce severe charge recombination for the improvement of PEC performance. Construction of heterojunction systems, such as Z-scheme and type II heterojunctions, could efficiently boost charge separation, whereas the mechanism of charge separation is still ambiguous.
View Article and Find Full Text PDFSemiconductor/co-catalyst coupling is considered as a promising strategy to enhance the photoelectrochemical (PEC) conversion efficiency. Unfortunately, this model system is faced with a serious interface recombination problem, which limits the further improvement of PEC performances. Here, a FeNiOOH co-catalyst with abundant oxygen vacancies on BiVO is fabricated through simple and economical NaBH reduction to accelerate hole transfer and achieve efficient electron-hole pair separation.
View Article and Find Full Text PDFPhotoelectrochemical (PEC) water splitting is an attractive strategy to convert and store of intermittent solar power into fuel energy. However, the detrimental charge recombination of photogenerated electrons and holes severely limits its efficiency. Despite electrocatalyst loading can obviously improve the PEC conversion efficiency, current systems still suffer from high recombination owing to the surface states.
View Article and Find Full Text PDFJ Colloid Interface Sci
April 2022
Activation of inert propylene to produce propylene oxide (PO) is critical, but still faces some challenges in realizing higher PO selectivity and productivity. Herein, a temperature-controlled phase transfer catalyst (MoOO·DMF) is prepared for the liquid-phase epoxidation of propylene with tert-butyl hydroperoxide (TBHP) as oxidant, which exhibit the selectivity of 90.6% and the productivity of 1286.
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