Very high concentrations of uranium (up to 4000 ppm) were found in a natural soil in the Dischma valley, an alpine region in the Grisons canton in Switzerland. The goal of this study was to examine the redox state and the nature of uranium binding in the soil matrix in order to understand the accumulation mechanism. Pore water profiles collected from Dischma soil revealed the establishment of anoxic conditions with increasing soil depth.
Rational design of metal single-site embedded porous graphitic carbon nitride (P-g-C 3 N 4 ) nanostructures exploiting maximum atom utilization is warranted to enhance the thermal CO oxidation (CO Ox ) reaction. Herein, a facile, green, one-pot, and template-free approach is developed to fabricate the hierarchical porous P-g-C 3 N 4 -crumpled ultrathin nanosheets atomically doped with copper single atoms (Cu−P-g-C 3 N 4 ). Mechanistically, the quick protonation of melamine and pyridine under acidic conditions induces deamination to form melem, which is polycondensed under heating. The interconnected pores, high surface area (240 m 2 g −1 ), and maximized exposed isolated Cu atomic active sites (1.8 wt %) coordinated with nitrogen atom P-g-C 3 N 4 are the salient features of Cu− P-g-C 3 N 4 that endowed complete conversion to CO 2 at 184 °C. In contrast, P-g-C 3 N 4 only converted 3.8% of CO even at 350 °C, implying the electronic effect of Cu single atoms. The abundant Cu-nitrogen moieties can drastically weaken the binding affinity of the CO-oxidation (CO Ox ) intermediates and products, thus accelerating the reaction kinetics at a low temperature. This study may promote the fabrication of P-g-C 3 N 4 doped with various single atoms for the oxidation of CO.
The reactivity in the selective catalytic reduction of the individual and binary components of NbO
x
−MnO
x
−CeO2 catalysts has been studied with coated cordierite monoliths in the temperature range of 150−450 °C. FTIRS, DRIFTS, TA, XRD, BET, and XAS have been used to elucidate the structural and catalytic properties. The results confirmed the contribution of the manganese oxides, particularly to the low-temperature NO-to-NO2 oxidation reaction. The significant increase of the surface acidity as a result of niobium oxide addition has been established. The data obtained revealed also the strong interaction between the manganese and niobium catalytic active sites. This phenomenon leads to a very good distribution of the oxidizing and acidic sites in the catalyst structure and also diminishes the unselective NH3 oxidation at higher temperatures. However, in order to keep the low-temperature catalytic activity, an excess of manganese relative to the niobium content is needed.
The SuperXAS beamline at the Swiss Light Source (SLS) features a permanently installed monochromator for quick scanning EXAFS (QEXAFS) spectroscopy in series with a conventional double crystal monochromator (DCM). All installed optical components like collimating and focussing mirrors can be used by both devices. The remote exchange of the monochromators is possible in less than five minutes while maintaining the beam geometry on the sample. The QEXAFS system allows fast absorption scans down to the millisecond range for the investigation of time dependent processes. Using a Si(111) channel cut crystal the energy range from 5-16 keV can be covered, with a Si(311) cut the range 9.5-30 keV. Usually a quick scanning interval of 0.1° -2° in Bragg angle is selected, thus covering XANES, full EXAFS or multiple edge scans of e.g. all L-edges of a heavy element. Up to about 80 spectra per second can be collected, corresponding to a time resolution of 12.5 ms. The high intensity of the beamline even facilitates fluorescence measurements on dilute samples.
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