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化工进展  2015 

富铈Ce1-xLaxO2催化甲烷氧氯化性能

DOI: 10.16085/j.issn.1000-6613.2015.12.018, PP. 4248-4253

Keywords: 甲烷,活化,氧化,Ce1-xLaxO2,氧氯化,氯甲烷

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Abstract:

以硝酸铈、硝酸镧为前体,用氨水共沉淀法制备了一系列Ce1-xLaxO2(x≤0.5)催化剂,利用XRD、N2吸附-脱附、SEM、Raman、H2-TPR和OSC对催化剂的物理化学性质进行了表征,并考察其在甲烷氧氯化反应中的催化性能。结果表明Ce1-xLaxO2催化剂的氧化还原性质随着镧含量的变化发生显著改变,并且这一性质的变化与反应的转化率及产物分布具有较强的联系。Ce1-xLaxO2表面氧物种的活泼性对催化剂活性影响显著,而体相氧物种容易将生成的甲烷氯化物深度氧化。在Ce1-xLaxO2(x0.8La0.2O2催化剂上氯甲烷选择性最高为52%。在体相氧物种更活泼的Ce0.7La0.3O2和Ce0.5La0.5O2上产物中CO的选择性显著上升,Ce0.5La0.5O2催化剂上CO选择性高达48%。稳定性测试表明Ce0.8La0.2O2催化剂具有良好的稳定性。

References

[1]  毕先钧,洪品杰,戴树珊. 甲烷部分氧化制合成气的研究[J]. 分子催化,1998,12(5):342-348.
[2]  Wei Yingxu,Zhang Dazhi,Liu Zhongmin,et al. Methl halide to olefins and gasoline over zeolites and SAPO catalysts:A new route of MTO and MTG[J]. Chinese Journal of Catalysis,2012,33(1):11-21.
[3]  Kunlun D,Alan R D,Aihua Z,et al. Hydrodebromination and oligomerization of dibromomethane[J]. ACS Catalysis,2012,2(4):479-486.
[4]  孔令涛,沈本贤,蒋章. 硅含量对氯甲烷制取低碳烯烃的SAPO-34分子筛酸性的影响[J]. 化工进展,2015,34(2):413-418.
[5]  Garcia C L,Resasco D E. Effect of the support and the addition of a second promoter on potassium chloride(II) chloride catalysts used in the oxychlorination of methane[J]. Applied Catalysis,1989,46(2):251-267.
[6]  Garcia C L,Resasco D E. High-temperature oxychlorination catalysts:Role of LaCl3 as an inhibitor of the segregation of active species duing heating/cooling cycles[J]. Journal of Catalysis,1990,122(1):151-165.
[7]  Peringer E,Podkolzin S G,Lercher J A,et al. LaCl3-based catalysts for oxidative chlorination of CH4[J]. Topics in Catalysis,2006,38(1-3):211-220.
[8]  Peringer E,Tejuja C,Lercher J A,et al. On the synthesis of LaCl3 catalysts for oxidative chlorination of methane[J]. Applied Catalysis A:General,2008,350(2):178-185.
[9]  Peringer E,Salzinger M,Lercher J A,et al. Modified lanthanum catalysts for oxidative chlorination of methane[J]. Topics in Catalysis,2009,52(9):1220-1231.
[10]  Shalygin A,Paukshtis E,Kovalyov E,et al. Light olefins synthesis from C1—C2 paraffins via oxychlorination process[J]. Frontiers of Chemical Science and Engineering,2013,7(3):279-288.
[11]  He J L,Xu T,Wang Y,et al. Transformation of methane to propylene:A two-step reaction route catalyzed by modified CeO2 nanocrystals and zeolites[J]. Angewandte Chemie,2012,124(10):2488-2492.
[12]  Hernandez W Y,Laguna O H,Centeno M A,et al. Structural and catalytic properties of lanthanide(La,Eu,Gd) doped ceria[J]. Journal of Solid state Chemistry,2011,184:3014-3020.
[13]  Reddy B M,Khan A. Recent advances on TiO2-ZrO2 mixed oxides as catalysts and catalyst supports[J]. Catalysis Reviews,2005,47(2):257-296.
[14]  Wang X,Rodriguez J A,Hanson J C,et al. Unusual physical and chemical properties of Cu in Ce1-xCuxO2 oxides[J]. Journal of Physical Chemistry B,2005,109(42):19595-19603.
[15]  Reddy B M,Katta L,Thrimurthulu G. Novel nanocrystalline Ce1-xLaxO2-delta (x=0.2) solid solutions:Structural characteristics and catalytic performance[J]. Chemistry of Matericals,2010,22(2):467-475.
[16]  Wang Y,Liang S,Cao A,et al. Au-mixed Lanthanum/cerium oxide catalysts for water gas shift[J]. Applied Catalysis B:Environment,2010,99(1-2):89-95.
[17]  杨伯伦,贺拥军. 西部天然气资源化工利用的思考与建议[J]. 化工进展,2001,20(6):1-6.
[18]  刘昌俊,许根慧. 一碳化工产品及其发展方向[J]. 化工学报,2003,54(4):524-531. 浏览
[19]  Lin R,Ding Y,Gong L,et al. Efficient and stable silica-supported iron phosphate catalysts for oxidative bromination of methane[J]. Journal of Catalysis,2010,272(1):65-73.
[20]  井强山,方林霞,娄辉,等. 甲烷临氧催化转化制合成气研究进 展[J]. 化工进展,2008,27(4):503-507. 浏览
[21]  李娟,吴良鹏,邱勇,等. 费托合成催化剂的研究进展[J]. 化工进展,2013,32(s1):100-109.

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