Transition metal (TM)-based bimetallic spinel oxides can efficiently activate peroxymonosulfate (PMS) presumably attributed to enhanced electron transfer between TMs,b ut the existing model cannot fully explain the efficient TM redoxc ycling. Here,w ed iscover ac ritical role of TM À O covalency in governing the intrinsic catalytic activity of Co 3Àx Mn x O 4 spinel oxides.E xperimental and theoretical analysis reveals that the Co sites significantly raises the Mn valence and enlarges MnÀOc ovalency in octahedral configuration, thereby lowering the charge transfer energy to favor Mn Oh-PMS interaction. With appropriate Mn IV /Mn III ratio to balance PMS adsorption and Mn IV reduction, the Co 1.1 Mn 1.9 O 4 exhibits remarkable catalytic activities for PMS activation and pollutant degradation, outperforming all the reported TM spinel oxides.T he improved understandings on the origins of spinel oxides activity for PMS activation may inspire the development of more active and robust metal oxide catalysts.
Orthorhombic V(2)O(5) single-crystalline nanobelts with widths of 100-300 nm, thicknesses of 30-40 nm, and lengths up to tens of micrometers have been synthesized on a large scale in a hydrogen peroxide aqueous solution by an environmentally friendly chemical route. Such nanobelts grow along the direction of [010]. The influence of the reaction time on the crystal structures and morphologies of the resulting products are investigated. A probable dehydration-recrystallization-cleavage mechanism for the formation of V(2)O(5) nanobelts is proposed. The experiments demonstrate that the use of a nanosized belt-like structure can considerably enhance the specific discharge capacity in lithium-ion batteries.
Removal of organic micropollutants from water through advanced oxidation processes (AOPs) is hampered by the excessive input of energy and/or chemicals as well as the large amounts of residuals resulting from incomplete mineralization. Herein, we report a new water purification paradigm, the direct oxidative transfer process (DOTP), which enables complete, highly efficient decontamination at very low dosage of oxidants. DOTP differs fundamentally from AOPs and adsorption in its pollutant removal behavior and mechanisms. In DOTP, the nanocatalyst can interact with persulfate to activate the pollutants by lowering their reductive potential energy, which triggers a non-decomposing oxidative transfer of pollutants from the bulk solution to the nanocatalyst surface. By leveraging the activation, stabilization, and accumulation functions of the heterogeneous catalyst, the DOTP can occur spontaneously on the nanocatalyst surface to enable complete removal of pollutants. The process is found to occur for diverse pollutants, oxidants, and nanocatalysts, including various low-cost catalysts. Significantly, DOTP requires no external energy input, has low oxidant consumption, produces no residual byproducts, and performs robustly in real environmental matrices. These favorable features render DOTP an extremely promising nanotechnology platform for water purification.
Single-crystal cerium hydroxide carbonate (Ce(OH)CO3) triangular microplates with the hexagonal phase have been successfully synthesized by a hydrothermal method at 150 degrees C using cerium nitrate (Ce(NO3)3.6H2O) as the cerium source, aqueous carbamide as both an alkaline and carbon source, and cetyltrimethylammonium bromide (CTAB) as a surfactant. Single-crystal ceria (CeO2) triangular microplates have been fabricated by a thermal decomposition-oxidation process at 650 degrees C for 7 h using single-crystal Ce(OH)CO3 microplates as the precursor. The shape of the Ce(OH)CO3 microplate was sustained after thermal decomposition-oxidation to CeO2. The products were characterized by X-ray powder diffraction (XRD), transmission electron microscopy (TEM), field-emission scanning electron microscopy (FE-SEM), differential scanning calorimetric analysis (DSC), and thermogravimetric analysis (TG).
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