CO 2 reforming of methane into syngas over Sm 2 O 3 -La 2 O 3 (SL)-supported Ni catalyst was investigated in a fixed-bed quartz reactor and the best catalytic activity was observed over Ni/SL (sol-gel) due to the reduction of the perovskite LaNiO 3 and spinel La 2 NiO 4 to form small nickel particles. The conversion of CH 4 and CO 2 over Ni/SL(sol-gel) were 55% and 57%, respectively, the selectivity of H 2 and CO were 96% and 98%, significantly higher than those over Ni/SL (imp) catalyst at 700 °C and a GHSV of 4.8 × 10 4 mL • h -1 • g -1 cat . In the meantime, the Sm 2 O 3 -La 2 O 3 -supported Ni catalysts were characterized by means of techniques, such as BET, XRD, H 2 -TPR, TG/DTA, HRTEM, XPS, and XAES.
A series of xMnyCe/hexagonal mesoporous silica (HMS) sorbents with wormhole-like structure was prepared by a sol−gel method, and their performance for hot coal gas desulfurization was investigated at 600 °C. All xMnyCe/HMS sorbents exhibited high breakthrough sulfur capacity, and the utilization of these sorbents was much higher than that of 10Mn/HMS. The breakthrough sulfur capacity over 4Mn1Ce/HMS sorbents was 121.7 mg of S/g of sorbent with the utilization of 82.4%. Such a behavior was maintained in eight consecutive desulfurization−regeneration cycles. The effects of the desulfurization temperature, H 2 concentration, and 7% steam on the performance of 4Mn1Ce/HMS were examined. The fresh, used, and regenerated samples were characterized by means of X-ray diffraction, N 2 adsorption, Fourier transform infrared absorption spectroscopy, and high-resolution transmission electron microscopy techniques. The results confirmed that the manganese oxide was dispersed highly on the HMS support because of the synergetic effects of manganese oxide and ceria oxide, and the wormhole-like structure in sorbents promoted the diffusion of H 2 S molecules. The Brunauer−Emmett−Teller results revealed that the wormhole-like mesoporous structure in sorbents remained intact even after the eighth successive desulfurization/regeneration cycle.
An industrial cylinder Ni-based catalyst, LaNiO x /ZSM-5 (φ ) 3 mm), was prepared by a sol-gel method, and its catalytic performance was investigated for CH 4 /CO 2 reforming reaction not only in laboratory scale but also in pilot plant scale. The result revealed that the conversion of CH 4 and CO 2 was 97% and 94%, respectively, at 850 °C and gas hour space velocity ) 1.3 × 10 3 h -1 and remained a constant in the 100 h range, whereas carbon yield was ca. 5%. The properties of the catalyst were characterized by means of techniques such as X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET) surface area, high-resolution transmission electron microscopy (HRTEM), temperature-programmed reduction (TPR), and temperature-programmed oxidation (TPO) and compared to those of La 2 NiO 4 /MCM-41 and La 2 NiO 4 /γ-Al 2 O 3 catalysts.
Corncob, a widespread and inexpensive natural resource in China, was used to prepare activated carbon (AC) by chemical activation with potassium hydroxide (KOH). The adsorption equilibrium and kinetics of H2, CH4, and CO2 on AC were investigated at different temperatures. Adsorption isotherms of H2, CH4, and CO2 were correlated with the Langmuir and Freundich equations, and the heat of adsorption was determined. It was revealed that the Freundich adsorption equation was more apt to describe the adsorption procedure of H2, CH4, and CO2 compared to the Langmuir equation. Two simplified kinetic models including pseudo-first-order and -second-order equations were used to evaluate the adsorption processes. The results indicated that the adsorption of H2, CH4, and CO2 could be described properly by a pseudo-second-order equation. The kinetic parameters of this model were calculated and discussed.
The improved deactivation kinetic model over mesoporous LaFeO3/MCM-41 sorbents for hot coal gas desulfurization was established with mass-transfer correlation based on elementary stoichiometric equation, which consisted of both the spatial and the time partial differential equations. MATLAB software was used to solve partial differential equations by means of forward finite differential method and to estimate kinetic parameters via nonlinear least-squares fitting. The rate constants k a and k d were obtained via aforementioned kinetic model over different LaFeO3/MCM-41 sorbents. The calculated results were in accordance with experimental data under various operating conditions. The kinetic model can be used successfully to predict the distributions of H2S concentration at different times and spatial positions within fixed-bed layers, compared to unreacted shrinking core model, random pore model, or grain model. It is of very great significance to obtain basical chemical engineering data for the design of new reactor. For 50%LF2/MCM-41 sorbent, the calculated apparent activation energy (E a) and deactivation energy (E d) for chemical reaction of LaFeO3 active sites are 32.1 and 15.1 kJ·mol–1, respectively, based on the experimental data of desulfurization process.
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