The Ni-loaded cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2) catalysts (xNi/OMS-2: x = 1, 3, 5, and 10 wt%) were prepared by a pre-incorporation method. Physicochemical properties of the as-synthesized materials were characterized by means of various techniques, and their catalytic activities for CO, ethyl acetate, and toluene oxidation were evaluated.The loading of Ni played an important role in improving physicochemical propertiesof OMS-2. Among all of the samples, 5Ni/OMS-2 exhibited the best catalytic activity, with the T90 being 155 °C for CO oxidation at a space velocity (SV) of 60,000 mL/(g·h), 225 °C for ethyl acetate oxidation at an SV of 240,000 mL/(g·h), and 300 °C for toluene oxidation at an SV of 240,000 mL/(g·h), which was due to its high Mn3+ content and Oads concentration, good low-temperature reducibility and lattice oxygen mobility, and strong interaction between the Ni species and the OMS-2 support. In addition, catalytic mechanisms of the oxidation of three pollutants over 5Ni/OMS-2 were also studied. The oxidation of CO, ethyl acetate, and toluene over the catalysts took place first via the activated adsorption, then intermediates formation, and finally complete conversion of the formed intermediates to CO2 and H2O.
Different Cu contents (x wt%) were supported on the cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2) (xCu/OMS-2; x = 1, 5, 15, and 20) via a pre-incorporation method. Physicochemical properties of the OMS-2 and xCu/OMS-2 samples were characterized by means of the XRD, FT-IR, SEM, TG/DTG, ICP-OES, XPS, O2-TPD, H2-TPR, and in situ DRIFTS techniques, and their catalytic activities were measured for the oxidation of CO, ethyl acetate, and toluene. The results show that the Cu species were homogeneously dispersed in the tunnel and framework structure of OMS-2. Among all of the samples, 15Cu/OMS-2 sample exhibited the best activities with the T50% of 65, 165, and 240 °C as well as the T90% of 85, 215, and 290 °C for CO, ethyl acetate and toluene oxidation, respectively, which was due to the existence of the Cu species and Mn3+/Mn4+ redox couples, rich oxygen vacancies, good oxygen mobility, low-temperature reducibility, and strong interaction between the Cu species and the OMS-2 support. The reaction mechanisms were also deduced by analyzing the in situ DRIFTS spectra of the 15Cu/OMS-2 sample. The excellent oxygen mobility associated with the electron transfer between Cu species and Mn3+/Mn4+ redox couples might be conducive to the continuous replenishment of active oxygen species and the constantly generated reactant intermediates, thereby increasing the reactant reaction rate.
The poisoning effects of alkali metals (K and Na) and alkaline earth metals (Ca and Mg) on catalytic performance of the 2Nb4Ce/Zr-PILC catalyst for the selective catalytic reduction of NOx with NH3 (NH3-SCR) were investigated, and physicochemical properties of the catalysts were characterized by means of the X-ray diffraction XRD (XRD), Brunner−Emmet−Teller (BET), hydrogen temperature-programmed reduction (H2-TPR), X-ray Photoelectron Spectroscopy (XPS), ammonia temperature-programmed desorption (NH3-TPD), and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) techniques. Doping of M (M = K, Na, Ca, and Mg) deactivated the 2Nb4Ce/Zr-PILC catalyst according to the sequence of 0.8 K > 0.8 Na > 0.8 Ca > 0.8 Mg (M/Ce molar ratio = 0.8). The characterization results showed that the decreases in redox ability, NH3 adsorption, Ce3+/Ce4+ atomic ratio, and amount of the chemisorbed oxygen (Oβ) were the important factors influencing catalytic activities of the alkali metal-and alkaline earth metal-doped samples. Consequently, compared with the Mg- and Ca-doped samples, doping of K caused the 2Nb4Ce/Zr-PILC sample to possess the lowest redox ability, NH3 adsorption, and amount of the Oβ species, which resulted in an obvious deactivation effect.
The reduced graphene oxide (rGO)-promoted α-MnO2 nanorods-supported Pt (xPt-yrGO/α-MnO2, x = 0.93 wt%, y = 0.5, 1.0, and 2.0 wt%) nanocatalysts were prepared using a polyvinyl alcohol (PVA)-protected reduction method. After an appropriate loading of Pt on α-MnO2, the strong metal–support interaction between Pt and α-MnO2 was beneficial for an increase in catalytic activity. The simultaneous addition of rGO to α-MnO2 not only provided a more amount of benzene adsorption sites, but also acted as an electron transfer channel to accelerate charge migration, thus further improving catalytic activity of α-MnO2. Among all of the catalyst samples, 0.94Pt-1.0rGO/α-MnO2 showed the best catalytic performance with 90% benzene conversion at 160 °C and a gas hourly space velocity (GHSV) of 60,000 mL/(g h), which was better than that over the other Pt-based catalysts. The results of in situ DRIFTS characterization revealed that phenol, benzoquinone, and carboxylate species were the intermediates and eventually oxidized to CO2 and H2O. When sulfur dioxide was present, catalytic activity of α-MnO2 decreased due to the formation of manganese sulfate that blocked the active sites, while the loading of Pt and rGO hindered the chemisorption of SO2 and prevented the active sites of the catalyst from being poisoned by SO2, thus enhancing sulfur resistance of the catalyst. The 0.94Pt-1.0rGO/α-MnO2 catalyst presented in this work can be considered as a cost-effective and promising catalyst for the oxidative removal of volatile organic compounds.
As a heavy metal, Pb is one component in coal-fired flue gas and is widely considered to have a strong negative effect on catalyst activity in the selective catalytic reduction of NOx by NH3 (NH3-SCR). In this paper, we investigated the deactivation mechanism of the Mo-Ce/Zr-PILC catalyst induced by Pb in detail. We found that NO conversion over the 3Mo4Ce/Zr-PILC catalyst decreased greatly after the addition of Pb. The more severe deactivation induced by Pb was attributed to low surface area, lower amounts of chemisorbed oxygen species and surface Ce3+, and lower redox ability and surface acidity (especially a low number of Brønsted acid sites). Furthermore, the addition of Pb inhibited the formation of highly active intermediate nitrate species generated on the surface of the catalyst, hence decreasing the NH3-SCR activity.
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