Pillared clays with Zr and Fe/Cu/Zr polycations have been prepared from natural clays found in large deposits of Kazakhstan and assessed as catalysts for the catalytic wet peroxide oxidation (CWPO), using 4-nitrophenol (4-NP) as model compound. The performance of the catalysts was followed by measuring the concentration of 4-NP, H2O2 and the total organic carbon (TOC), considering C4-NP = 5 g L-1 , CH 2 O 2 = 17.8 g L-1 , Ccat = 2.5 g L-1 , initial pH = 3.0 and T = 50°C. At those selected conditions, the pillared clays showed higher activity than natural clays in the CWPO of 4-NP. The conversion of the model pollutant was complete when Fe/Cu/Zr-PILCs were used, with the TOC removal reaching 78.4% after 24 h with the best Fe/Cu/Zr-PILC. The H2O2, 4-NP and TOC time-evolution was well described by a kinetic model based on TOC lumps in three blocks, considering the initial TOC (corresponding to 4-NP), the production of oxidizable intermediates and the formation of refractory products.
Many pharmaceuticals have been recently identified at trace levels worldwide in the aquatic environment. Among them, the highly consumed paracetamol (PCM), an analgesic and antipyretic drug, is largely being accumulated in the aquatic environment due to inefficient removal by conventional sewage treatment plants. This work deals with the treatment of PCM, used as a model pharmaceutical contaminant of emerging concern, by catalytic wet peroxide oxidation using clay-based materials as catalysts. The catalysts were prepared from natural clays, extracted from four different deposits using acid-activated treatment, calcination, and pillarization with Fe and Co. Pillared clays show the highest catalytic activity owing to the presence of metals, allowing to remove completely the PCM after 6 h under the following operating conditions: CPCM = 100 mg L−1, CH2O2 = 472 mg L−1, Ccat = 2.5 g L−1, initial pH = 3.5 and T = 80 °C. The prepared materials presented high stability since leached iron was measured at the end of reaction and found to be lower than 0.1 mg L−1.
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Ethanol steam reforming catalyst’s precursors, i.e., nanocomposites of complex oxides with the general formula [Pr0.15Sm0.15Ce0.35Zr0.35O2 + LaMn0.45Ni0.45Ru0.1O3] (1:1 by mass), were synthesized by three different methods. It was shown that two synthesis methods – ultrasonic dispersion and sequential polymeric method, lead to the formation of the nanocomposite perovskite–fluorite system with the specific surface area up to 50 m2/g. Reduction of samples at 400–500°C lead to the formation of Ni–Ru alloy nanoparticles strongly bound with the surface of oxide nanocomposite. Catalytic tests in ethanol steam reforming reaction at 500–600°C showed the highest specific activity of the sample prepared by the sequential polymeric method due to the location of Ni- and Ru-containing perovskite mainly on the surface of the composite providing a high concentration of active metal centers. At higher temperatures for all samples, ethanol conversion approached 100% with hydrogen yield varying in the range of 65–75%. A study of spent catalysts confirmed the absence of carbon deposits after long-term catalytic tests at 650°C.
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