Synthesis gas production using oxygen storage materials as oxygen carrier over circulating fluidized bed

A novel process for synthesis gas production over Circulating Fluidized Bed （CFB） using oxygen storage materials as oxygen carder was reported. First, oxygen in the air was chemically fixed and converted to lattice oxygen of oxygen storage materials over regenerator, and then methane was selectively oxidized to synthesis gas with lattice oxygen of oxygen storage materials over riser reactor. The results from simulation reaction of CFB by sequential redox reaction on a fixed bed reactor using lanthanum-based perovskite LaFeO3 and La0.8Sr0.2Fe0.9CO0.1O3 oxides prepared by sol-gel, suggested that the depleted oxygen species could be regenerated, and methane could be oxidized to synthesis gas by lattice oxygen with high selectivity. The partial oxidation of methane to synthesis gas over CFB using lattice oxygen of the oxygen storage materials instead of gaseous oxygen should be possibly applicable.

Dynamic Oxygen Storage Capacity Measurements on Ceria-Based Material

Dynamic oxygen storage and release capability （OSC） measurement apparatus was designed to evaluate the OSC performance of ceria-based oxygen storage material. The optimum measurement condition was at a frequency of 0.1 Hz with the inlet gas-flow sequence CO （5S）→O2（5S）→CO→O2 and a flow rate of 300 ml·min^-1. Under this condition, similar regular square wave in the inlet and outlet of the reactor was obtained to guarantee the reliability of the dynamic OSC results. The dynamic OSC performance of the CeO2 and Ce0.67Zr0.33O2 mixed oxide prepared using the citric sol-gel method was studied at the optimum measurement condition with focus on both quantitative and qualitative analyses, The results reveal distinctly that Ce0.67Zr0.33O2 had better dynamic OSC performance because of its higher oxygen migration rate than CeO2. Under dynamic conditions, two CO2 production peaks occurred corresponding to the CO pulse and the O2 pulse, respectively, during the entire cycle. The intensity and ratio between the two CO2 productions were highly influenced by temperature and frequency indicating complex surface phenomena during the oxygen storage/release process, As a result, this set-up can be applied to the evaluation of ceria-based material on the OSC performance.

Effect of doping elements on catalytic performance of CeO_2-ZrO_2 solid solutions

CeZr, CeYZr, LaCeZr, LaCePrZr, LaCePrYZr, and LaCePr solid solutions were prepared via the coprecipitation method, and characterized by means of X-Ray Diffraction （XRD） and Brunauer-Emmett-Teller （BET） techniques. The oxygen storage capacity （OSC） of the solid solutions was evaluated by the pulse technique and the catalytic activity was assessed using a 4-channel catalysis device. It was seen that the solid solutions presented cubic structure. The specific surface area and thermal stability could be enhanced by doping Y into the solid solutions. Doping a small amount of La had a positive effect on the thermal durability while doping a large amount of La decreased the specific surface area and the thermal stability. LaCePrZr and LaCePrYZr solid solutions synthesized using Baotou rare earth mineral residue enriched with LaCePr after Nd extraction presented a certain higher value in specific surface area and thermal stability, thereby enabling to be used as economic catalysts for automobile exhaust purification. Coating Al2O3 or SiO2 layer on the surface of ceria-zirconia solid solutions increased the specific surface area and thermal resistance.

SO_(4)^(2-)-modified La,Y-doped ceria-zirconia with high oxygen storage capacity and its application in Pd-only three-way catalysts

As the oxygen redox ability shows great effects on the catalytic performances of ceria-zirconia based materials,many strategies have been utilized to improve the oxygen storage capacity.Here in this study,we report a simple and facile approach to prepare a SO_(4)^(2-)-modified La,Y-doped ceria-zirconia material(SO/CZLY-f)with high oxygen storage capacity.Due to the additional redox process between SO_(4)^(2-)and S^(2-),oxygen storage capacity of SO/CZLY-f(745.3μmol O_(2)/g)is about 1.6 times higher than that of La,Ydoped ceria-zirconia material without SO_(4)^(2-)modification.Moreover,the catalytic activities and stability of the corresponding Pd-only three-way catalyst were measured.Compared to that of Pd@CZLY-f,the operation window of CO,full conversion temperature of HC and NO over Pd@SO/CZLY-f are obviously widened and lowered,respectively.After aging treatment at 1100℃for 4 h,the superiority of aged Pdloading composite is still maintained.

Effects of ceria/zirconia ratio on properties of mixed CeO_2-ZrO_2-Al_2O_3 compound

A series of CexZr0.50-xAl0.50O1.75(0.05≤x≤0.45) mixed oxides with different Ce/Zr ratio were prepared by co-precipitation method and characterized by means of X-ray diffraction(XRD),Brunauer-Emmet Teller method(BET),temperature-programmed reduction(H2-TPR) and oxygen pulsing technique.The XRD results showed that all samples kept the single CeO2 cubic fluorite structure after calcination at 600 and 1000 oC for 5 h.The results of BET revealed that CexZr0.50-xAl0.50O1.75 with Ce/Zr molar ratio 1/1 exhibited hi...

Effect of Metal Oxide Doping into Ce_(0.5)Zr_(0.5)O_2 on Catalytic Activity of MnO_x/γ-Al_2O_3/Ce_(0.45)Zr_(0.45)M_(0.1)O_x (M=Y, La, Mn) Honeycomb Catalysts

This article showed that the catalytic activity of MnOx/γ-Al2O3/Ce0.5Zr0.5O2 monolithic catalyst toward the catalytic combustion of ethanol in a fixed bed reactor could be greatly improved by doping three metal oxides into Ce0.5Zr0.5O2. The catalytic activity of MnOx/γ-Al2O3/Ce0.45Zr0.45M0.1 Ox （M = Y, La, Mn） is better than that of MnOx/γ-Al2O3/Ce0.5 Zr0.5O2. The order of activity of the catalysts is as follows： MnOx/γ-Al2O3/Ce0.45Zr0.45Y0.1Ox 〉 MnOc/γ-Al2O3/Ce0.45 Zr0.45La0.1Ox 〉 MnOx/γT-Al2O3/Ce0.45Zr0.45Mn0.1Ox 〉 MnOx/y-Al2O3/Ce0.5Zr0.5O2. The influence of the loading amount of manganese oxide in enhancing the catalytic activity of MnOx/γ-Al2O3/Ce0.45Zr0.45Y0.1 Ox was investigated. The results showed that when MnO2 loading amount was 10% （mass fraction）, the MnOx/Al2O3/Ce0.45Zr0.45Y0.1Ox catalyst recorded the highest activity.

Monolithic Catalysts with Low Noble-Metal Content for Exhaust Purification of Small Gasoline Engines

A series of low noble-metal coment monolithic catalysts for exhaust purification of small gasoline engines was investigated, and it was found that the Pt/Rh-OSM/Al2O3 （where OSM was oxygen storage material） catalyst with Ce0.5Zr0.5-MnOx（3%MnOx） OSM held low light-off temperature for CO, HC, and NO; quite wide three-way window, and outstanding thermal stability. The catalyst could efficiently comrol exhaust emission of small gasoline engines.

Low Temperature Catalytic Combustion of Ethanol over Pt/γ-Al_2O_3/Ce_xZr_(1-x)O_2 Honeycomb Catalysts

It has been found that the catalytic activity toward the decomposition of ethanol in a fix bed reactor can be greatly improved by loading Pt on the surface of CexZr1-xO2. In this study, we have investigated the effects of different x of Pt/γ-Al2O3/CexZr1-xO2 on the catalytic activity of catalysts. The prepared catalysts were characterized by BET, XRD, and TPR. The BET surface areas of the catalysts decreased with x decreasing. XRD results reveal that deposited Pt dispersed on the CexZr1-xO2 and γ-Al2O3 matrix. The order of catalytic activities is Pt/γ-Al2O3/ Ce0.5Zr0.5O2〉Pt/γ-Al2O3/Ce0.25Zr0.75O2〉Pt/γ-Al2O3/Ce0.75Zr0.26O2〉Pt/γ-Al2O3/CeO2〉Pt/γ-Al2O3/ZrO2. Among the catalysts, the reduction peak area of Pt/γ-Al2O3/Ce0.5Zr0.5O2 is the largest and the oxygen mobility is noticeably promoted, which is in good harmony with the catalytic activity. Incorporation of ZrO2 into the CeO2 lattice considerably decreases the destruction temperature for ethanol. Based on these observations, the mechanistic role of oxygen mobility in the oxidation reaction has been suggested.

A simple and novel effective strategy using mechanical treatment to improve the oxygen uptake/release rate of YBaCo_(4)O_(7+δ) for thermochemical cycles

In recent years,oxygen storage materials(OSMs)have been widely used in many fields.It would be particularly important for researchers to design high-oxygen-uptake/release-rate materials.In this study,various synthesis processes were used to successfully synthesize YBaCo_(4)O_(7+δ)and comprehensively investigate their potential applications.Compa red with traditional solid-state reaction method and co-precipitation method,the results demonstrated that the utilization of mechanical ball milling treatment on co-precipitated precursors could lead to samples with reversible oxygen uptake/release under an oxidative atmosphere at low temperatures.The resultant materials exhibited fast oxygen absorption/desorption rate that could uptake/release oxygen directly to the equilibrium state within 9 min and20 min,respectively.The mechanochemically ball-milled sample possessed outstanding oxygen sto rage performance,which could be attributed to their small particle size,the active outer surface of particles,large specific surface area,and relatively low activation energy.Moreover,the ball-milled sample also exhibited excellent cycling stability during relatively short time spacing.TG results also demonstrated that the ball-milled samples could reversibly uptake/release 2.90 wt.%of excess oxygen(while only 0.70 wt.%for solid-state samples)by adjusting the ambient temperature under pure O_(2) atmosphere,which would make them promising candidates in various applications.This research demonstrated that mechanical treatment could be an effective strategy to tune the properties and oxygen storage capacity(OSC)performances of YBaCo_(4)O_(7+δ).