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水热法制备 La(1-x)Sr(x)M(1-y)Fe(y)O(3) (M = Mn, Co)及其对甲苯去除的高催化活性

Hydrothermal fabrication and catalytic properties of La(1-x)Sr(x)M(1-y)Fe(y)O(3) (M = Mn, Co) that are highly active for the removal of toluene.

机构信息

Laboratory of Catalysis Chemistry and Nanoscience, Department of Chemistry and Chemical Engineering, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing, People's Republic of China.

出版信息

Environ Sci Technol. 2010 Apr 1;44(7):2618-23. doi: 10.1021/es9031997.

Abstract

A series of La(1-x)Sr(x)M(1-y)Fe(y)O(3) (M = Mn, Co; x = 0, 0.4; y = 0.1, 1.0) perovskite-type oxide catalysts have been fabricated via a strategy of citric acid complexation coupled with hydrothermal treatment. The materials are characterized by a number of analytical techniques. The oxidation of toluene is used as a probe reaction for the evaluation of catalytic performance. It is found that both La(0.6)Sr(0.4)FeO(3) and LaFeO(3) exhibit high activities. The partial substitution of manganese and cobalt with iron can significantly improve the catalytic performance of La(0.6)Sr(0.4)MnO(3) and La(0.6)Sr(0.4)CoO(3). At toluene/O(2) molar ratio = 1/200 and space velocity = 20,000 h(-1), the catalytic activity decreases in the sequence of La(0.6)Sr(0.4)Co(0.9)Fe(0.1)O(3) > La(0.6)Sr(0.4)FeO(3) > La(0.6)Sr(0.4)Mn(0.9)Fe(0.1)O(3) > LaFeO(3) > La(0.6)Sr(0.4)CoO(3) > La(0.6)Sr(0.4)MnO(3). Compared to the Fe-free counterparts, the La(0.6)Sr(0.4)Mn(0.9)Fe(0.1)O(3) and La(0.6)Sr(0.4)Co(0.9)Fe(0.1)O(3) catalysts are, respectively, 50 and 85 degrees C lower with regard to the temperature required for complete toluene oxidation. Toluene can be completely oxidized at 245 degrees C over La(0.6)Sr(0.4)Co(0.9)Fe(0.1)O(3). The excellent catalytic performance of La(0.6)Sr(0.4)Co(0.9)Fe(0.1)O(3) can be attributed to the presence of (i) Fe(3+)-O-Fe(4+) couples, (ii) a transition of electronic structure, and (iii) a trace amount of Co(3)O(4).

摘要

一系列的 La(1-x)Sr(x)M(1-y)Fe(y)O(3)(M = Mn,Co;x = 0,0.4;y = 0.1,1.0)钙钛矿型氧化物催化剂通过柠檬酸络合与水热处理相结合的策略制备。通过多种分析技术对材料进行了表征。甲苯氧化被用作评价催化性能的探针反应。结果发现,La(0.6)Sr(0.4)FeO(3)和 LaFeO(3)都表现出很高的活性。用铁部分取代锰和钴可以显著提高 La(0.6)Sr(0.4)MnO(3)和 La(0.6)Sr(0.4)CoO(3)的催化性能。在甲苯/O(2)摩尔比= 1/200 和空间速度= 20,000 h(-1)下,催化活性按 La(0.6)Sr(0.4)Co(0.9)Fe(0.1)O(3)>La(0.6)Sr(0.4)FeO(3)>La(0.6)Sr(0.4)Mn(0.9)Fe(0.1)O(3)>LaFeO(3)>La(0.6)Sr(0.4)CoO(3)>La(0.6)Sr(0.4)MnO(3)的顺序降低。与不含铁的对应物相比,La(0.6)Sr(0.4)Mn(0.9)Fe(0.1)O(3)和 La(0.6)Sr(0.4)Co(0.9)Fe(0.1)O(3)催化剂分别在完全氧化甲苯所需的温度下低 50 和 85°C。La(0.6)Sr(0.4)Co(0.9)Fe(0.1)O(3)可在 245°C下完全氧化甲苯。La(0.6)Sr(0.4)Co(0.9)Fe(0.1)O(3)优异的催化性能可归因于以下几点:(i)Fe(3+)-O-Fe(4+)偶对,(ii)电子结构的转变,以及(iii)痕量的 Co(3)O(4)。

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