Selective oxidation of methane and carbon deposition over Fe_2O_3/Ce_(1-x)Zr_xO_2 oxides

A series of Fe2O3/Al2O3, Fe2O3/CeO2, Ce0.7Zr0.3O2, and Fe2O3/Ce1-xZrxO2（x = 0.1–0.4） oxides was prepared and their physicochemical features were investigated by X-ray diffraction（XRD）, transmission electron microscope（TEM）, and H2-temperature-programmed reduction（H2-TPR） techniques. The gas–solid reactions between these oxides and methane for syngas generation as well as the catalytic performance for selective oxidation of carbon deposition in O2-enriched atmosphere were investigated in detail. The results show that the samples with the presence of Fe2O3show much higher activity for methane oxidation compared with the Ce0.7Zr0.3O2solid solution,while the CeO2-contained samples represent higher CO selectively in methane oxidation than the Fe2O3/Al2O3sample. This suggests that the iron species should be the active sites for methane activation, and the cerium oxides provide the oxygen source for the selective oxidation of the activated methane to syngas during the reaction between methane and Fe2O3/Ce0.7Zr0.3O2. For the oxidation process of the carbon deposition, the CeO2-containing samples show much higher CO selectivity than the Fe2O3/Al2O3sample, which indicates that the cerium species should play a very important role in catalyzing the carbon selective oxidation to CO. The presence of the Ce–Zr–O solid solution could induce the growth direction of the carbonfilament, resulting in a loose contact between the carbon filament and the catalyst. This results in abundant exposed active sites for catalyzing carbon oxidation, strongly improving the oxidation rate of the carbon deposition over this sample. In addition, the Fe2O3/Ce0.7Zr0.3O2also represents much higher selectivity（ca. 97 %） for the conversion of carbon to CO than the Fe2O3/CeO2sample, which can be attributed to the higher concentration of reduced cerium sites on this sample. The increase of the Zr content in the Fe2O3/Ce1-xZrxO2samples could improve the reactivity of the materials for methane oxidation, but it also reduces the selectivity for CO formation.

Structure and catalytic property of CeO_2-ZrO_2-Fe_2O_3 mixed oxide catalysts for diesel soot combustion: Effect of preparation method

A series of Ceo.sFeo.30Zr0.20O2 catalysts were prepared by different methods （co-precipitations method, citric acid sol-gel method, impregnation method, physical mixed method, and hydrotherrnal method） and characterized by X-ray diffraction （XRD）, Raman spectroscopy, Brunauer-Emmett-Teller （BET） and H2-TPR measurements. Potential of the catalysts in the soot oxidation was evaluated in a temperature-programmed oxidation （TPO） apparatus. The results showed that all the Fe3＋ and Zr4＋ were incor- porated into ceria lattice to form a pure Ce-Fe-Zr-O solid solution for the co-precipitation sample, but two kinds of Fe phases ex- isted in the Ce-Fe-Zr-O catalysts prepared by other methods： Fe3＋ incorporated into CeO2 lattice and dispersed Fe2O3 clusters. The free Fe2O3 clusters could improve the activity of catalysts for soot oxidation comparing with the pure Ce-Fe-Zr-O solid solution owing to the synergetic effect between free Fe2O3 and surface oxygen vacancies. In addition, the activity of catalysts strongly relied on the surface reducibility of free Fe2O3 particles. Holding both abundant free Fe2O3 particles and high oxygen vacancy concentration, the hydrothermal Ce0.5Fe0.3Zr0.202 catalyst presented the lowest Ti （251℃, ignition temperature of soot oxidation） and Tm （310 ℃, maximum oxidation rate temperature） for soot combustion （with tight-contact between soot and catalysts） among the five samples. Even after aging at 800 ℃ for 10 h, the Ti and Tm were still relatively low, at 273 and 361 ℃, respectively, indicating high catalytic stability.

Achieving high conversion of syngas to aromatics

Realizing high CO conversion and high aromatics selectivity simultaneously in syngas-to-aromatics(STA)reaction is still challenging.Herein,we report a 57.5%CO conversion along with 74%aromatics selectivity over a composite catalyst consisting of Fe/ZnCr_(2)O_(4)(Fe modified ZnCr_(2)O_(4)spinel)oxide and H-ZSM-5 zeolite.Impregnation of only 3 wt%of Fe onto ZnCr_(2)O_(4)can remarkably increase CO conversion without sacrificing the aromatics selectivity.Oxygen vacancy concentration is improved after impregnating Fe.The highly dispersed iron carbide species is formed during the reaction over Fe/ZnCr_(2)O_(4)spinel oxide.The synergistic effect of oxygen vacancy and iron carbide results in a rapid formation of abundant oxygenated intermediate species,which can be continuously transformed to aromatics in H-ZSM-5.This study provides a new insight into the design of highly efficient catalyst for syngas conversion.

Effects of different sludge disintegration methods on sludge moisture distribution and dewatering performance

A key step in sludge treatment is sludge dewatering. However, activated sludge is generally very difficult to be dewatered. Sludge dewatering performance is largely affected by the sludge moisture distribution. Sludge disintegration can destroy the sludge structure and cell wall, so as change the sludge floc structure and moisture distribution, thus affecting the dewatering performance of sludge. In this article, the disintegration methods were ultrasound treatment, K2 Fe O4oxidation and KMn O4 oxidation. The degree of disintegration（DDCOD）, sludge moisture distribution and the final water content of sludge cake after centrifuging were measured. Results showed that three disintegration methods were all effective, and K2 Fe O4oxidation was more efficient than KMn O4 oxidation. The content of free water increased obviously with K2 Fe O4and KMn O4 oxidations, while it decreased with ultrasound treatment. The changes of free water and interstitial water were in the opposite trend. The content of bounding water decreased with K2 Fe O4oxidation, and increased slightly with KMn O4 oxidation, while it increased obviously with ultrasound treatment. The water content of sludge cake after centrifuging decreased with K2 Fe O4oxidation, and did not changed with KMn O4 oxidation, but increased obviously with ultrasound treatment. In summary, ultrasound treatment deteriorated the sludge dewaterability, while K2 Fe O4and KMn O4 oxidation improved the sludge dewaterability.