注册 English

Fe/SiO2纳米复合物上合成气制低碳烯烃催化性能研究

位健 ,  马现刚 ,  方传艳 ,  葛庆杰 ,  徐恒泳

downloadPDF
引用本文: 位健, 马现刚, 方传艳, 葛庆杰, 徐恒泳. Fe/SiO2纳米复合物上合成气制低碳烯烃催化性能研究[J]. 燃料化学学报, 2014, 42(7): 827-832. shu
Citation:  WEI Jian, MA Xian-gang, FANG Chuan-yan, GE Qing-jie, XU Heng-yong. Iron-silica nanocomposites as a catalyst for the selective conversion of syngas to light olefins[J]. Journal of Fuel Chemistry and Technology, 2014, 42(7): 827-832. shu

Fe/SiO2纳米复合物上合成气制低碳烯烃催化性能研究

    通讯作者: 葛庆杰,E-mail:geqj@dicp.ac.cn。
摘要: 分别采用一步合成法和常规共沉淀法制备了Fe/SiO2催化剂,通过N2物理吸附、X射线衍射、透射电镜、傅里叶变换红外光谱和程序升温还原等方法对催化剂进行了表征,并在固定床反应器中对其费托合成制低碳烯烃的催化性能进行了评价。结果表明,与共沉淀铁基催化剂不同,采用一步合成法制备的纳米复合物主要由Fe3O4相构成,形貌呈规则球形,平均粒径为30 nm,尺寸分布窄,更容易还原。一步合成法制得的Fe/SiO2催化剂对费托合成反应具有较高的活性和低碳烯烃选择性、较低的甲烷选择性和良好的稳定性。

English

  • 

    1. [1] 杨学萍, 董丽. 合成气直接制低碳烯烃技术进展与经济性分析[J]. 化工进展, 2012, 31(8): 1726-1731. (YANG Xue-ping, DONG Li. Technical progress and economical ananysis on the direct production of light olefins from syngas[J]. Chemical Industry and Engineering Progress, 2012, 31(8): 1726-1731.)[1] 杨学萍, 董丽. 合成气直接制低碳烯烃技术进展与经济性分析[J]. 化工进展, 2012, 31(8): 1726-1731. (YANG Xue-ping, DONG Li. Technical progress and economical ananysis on the direct production of light olefins from syngas[J]. Chemical Industry and Engineering Progress, 2012, 31(8): 1726-1731.)

    2. [2] TORRES GALVIS H M, DE JONG K P. Catalysts for production of lower olefins from synthesis gas[J]. ACS Catal, 2013, 3(9): 2130-2149.[2] TORRES GALVIS H M, DE JONG K P. Catalysts for production of lower olefins from synthesis gas[J]. ACS Catal, 2013, 3(9): 2130-2149.

    3. [3] DE SMIT E, WECKHUYSEN B M. The renaissance of iron-based Fischer-Tropsch synthesis: On the multifaceted catalyst deactivation behaviour[J]. Chem Soc Rev, 2008, 37(12): 2758-2781.[3] DE SMIT E, WECKHUYSEN B M. The renaissance of iron-based Fischer-Tropsch synthesis: On the multifaceted catalyst deactivation behaviour[J]. Chem Soc Rev, 2008, 37(12): 2758-2781.

    4. [4] ABELLO S, MONTANE D. Exploring iron-based multifunctional catalysts for Fischer-Tropsch synthesis[J]. ChemSusChem, 2011, 4(11): 1538-1556.[4] ABELLO S, MONTANE D. Exploring iron-based multifunctional catalysts for Fischer-Tropsch synthesis[J]. ChemSusChem, 2011, 4(11): 1538-1556.

    5. [5] MCDONALD M A, STORM D, BOUDART M. Hydrocarbon synthesis from CO-H2 on supported iron: Effect of particle size and interstitials[J]. J Catal, 1986, 102(2): 386-400.[5] MCDONALD M A, STORM D, BOUDART M. Hydrocarbon synthesis from CO-H2 on supported iron: Effect of particle size and interstitials[J]. J Catal, 1986, 102(2): 386-400.

    6. [6] BOUDART M, MCDONALD M A. Structure sensitivity of hydrocarbon synthesis from carbon monoxide and hydrogen[J]. J Phys Chem, 1984, 88(11): 2185-2195.[6] BOUDART M, MCDONALD M A. Structure sensitivity of hydrocarbon synthesis from carbon monoxide and hydrogen[J]. J Phys Chem, 1984, 88(11): 2185-2195.

    7. [7] DEN BREEJEN J P, SIETSMA J R A, FRIEDRICH H, BITTER J H, DE JONG K P. Design of supported cobalt catalysts with maximum activity for the Fischer-Tropsch synthesis[J]. J Catal, 2010, 270(1): 146-152.[7] DEN BREEJEN J P, SIETSMA J R A, FRIEDRICH H, BITTER J H, DE JONG K P. Design of supported cobalt catalysts with maximum activity for the Fischer-Tropsch synthesis[J]. J Catal, 2010, 270(1): 146-152.

    8. [8] 马利海, 张建利, 范素兵, 赵天生. 水热法Fe-Mn催化剂制备及其合成气制低碳烯烃催化活性[J]. 燃料化学学报, 2013, 41(11): 1356-1360. (MA Li-hai, ZHANG Jian-li, FAN Su-bing, ZHAO Tian-sheng. Preparation of Fe-Mn catalyst by hydrothermal methodand its catalytic activity for the synthesis of light olefins from CO hydrogenation[J]. Journal of Fuel Chemistry and Technology, 2013, 41(11): 1356-1360.)[8] 马利海, 张建利, 范素兵, 赵天生. 水热法Fe-Mn催化剂制备及其合成气制低碳烯烃催化活性[J]. 燃料化学学报, 2013, 41(11): 1356-1360. (MA Li-hai, ZHANG Jian-li, FAN Su-bing, ZHAO Tian-sheng. Preparation of Fe-Mn catalyst by hydrothermal methodand its catalytic activity for the synthesis of light olefins from CO hydrogenation[J]. Journal of Fuel Chemistry and Technology, 2013, 41(11): 1356-1360.)

    9. [9] KANG S H, BAE J W, SAI PRASAD P S, PARK S J, WOO K J, JUN K W. Effect of preparation method of Fe-based Fischer-Tropsch catalyst on their light olefin production[J]. Catal Lett, 2009, 130(3/4): 630-636.[9] KANG S H, BAE J W, SAI PRASAD P S, PARK S J, WOO K J, JUN K W. Effect of preparation method of Fe-based Fischer-Tropsch catalyst on their light olefin production[J]. Catal Lett, 2009, 130(3/4): 630-636.

    10. [10] LAURENT S, FORGE D, PORT M, ROCH A, ROBIC C, VANDER ELST L, MULLER R N. Magnetic iron oxide nanoparticles: Synthesis, stabilization, vectorization, physicochemical characterizations, and biological applications[J]. Chem Rev, 2008, 108(6): 2064-2110.[10] LAURENT S, FORGE D, PORT M, ROCH A, ROBIC C, VANDER ELST L, MULLER R N. Magnetic iron oxide nanoparticles: Synthesis, stabilization, vectorization, physicochemical characterizations, and biological applications[J]. Chem Rev, 2008, 108(6): 2064-2110.

    11. [11] GOLE A, STONE J W, GEMMILL W R, ZUR LOYE H C, MURPHY C J. Iron oxide coated gold nanorods: Synthesis, characterization, and magnetic manipulation[J]. Langmuir, 2008, 24(12): 6232-6237.[11] GOLE A, STONE J W, GEMMILL W R, ZUR LOYE H C, MURPHY C J. Iron oxide coated gold nanorods: Synthesis, characterization, and magnetic manipulation[J]. Langmuir, 2008, 24(12): 6232-6237.

    12. [12] XIONG Y, YE J, GU X, CHEN Q W. Synthesis and assembly of magnetite nanocubes into flux-closure rings[J]. J Phys Chem C, 2007, 111(19): 6998-7003.[12] XIONG Y, YE J, GU X, CHEN Q W. Synthesis and assembly of magnetite nanocubes into flux-closure rings[J]. J Phys Chem C, 2007, 111(19): 6998-7003.

    13. [13] RODULFO-BAECHLER S M, GONZÁ LEZ-CORTÉS S L, OROZCO J, SAGREDO V, FONTAL B, MORA A J, DELGADO G. Characterization of modified iron catalysts by X-ray diffraction, infrared spectroscopy, magnetic susceptibility and thermogravimetric analysis[J]. Mater Lett, 2004, 58(20): 2447-2450.[13] RODULFO-BAECHLER S M, GONZÁ LEZ-CORTÉS S L, OROZCO J, SAGREDO V, FONTAL B, MORA A J, DELGADO G. Characterization of modified iron catalysts by X-ray diffraction, infrared spectroscopy, magnetic susceptibility and thermogravimetric analysis[J]. Mater Lett, 2004, 58(20): 2447-2450.

    14. [14] ZHANG C H, WAN H J, YANG Y, XIANG H W, LI Y W. Study on the iron-silica interaction of a co-precipitated Fe/SiO2 Fischer-Tropsch synthesis catalyst[J]. Catal Commun, 2006, 7(9):733-738.[14] ZHANG C H, WAN H J, YANG Y, XIANG H W, LI Y W. Study on the iron-silica interaction of a co-precipitated Fe/SiO2 Fischer-Tropsch synthesis catalyst[J]. Catal Commun, 2006, 7(9):733-738.

    15. [15] SUO H Y, WANG S G, ZHANG C H, XU J, WU B S, YANG Y, XIANG H W, LI Y W. Chemical and structural effects of silica in iron-based Fischer-Tropsch synthesis catalysts[J]. J Catal, 2012, 286: 111-123.[15] SUO H Y, WANG S G, ZHANG C H, XU J, WU B S, YANG Y, XIANG H W, LI Y W. Chemical and structural effects of silica in iron-based Fischer-Tropsch synthesis catalysts[J]. J Catal, 2012, 286: 111-123.

    16. [16] JOZWIAK W K, KACZMAREK E, MANIECKI T P, IGNACZAK W, MANIUKIEWICZ W. Reduction behavior of iron oxides in hydrogen and carbon monoxide atmospheres[J]. Appl Catal A: Gen, 2007, 326(1): 17-27.[16] JOZWIAK W K, KACZMAREK E, MANIECKI T P, IGNACZAK W, MANIUKIEWICZ W. Reduction behavior of iron oxides in hydrogen and carbon monoxide atmospheres[J]. Appl Catal A: Gen, 2007, 326(1): 17-27.

    17. [17] REDL F X, BLACK C T, PAPAEFTHYMIOU G C, SANDSTROM R L, YIN M, ZENG H, MURRAY C B, O'BRIEN S P. Magnetic, electronic, and structural characterization of nonstoichiometric iron oxides at the nanoscale[J]. J Am Chem Soc, 2004, 126(44): 14583-14599.[17] REDL F X, BLACK C T, PAPAEFTHYMIOU G C, SANDSTROM R L, YIN M, ZENG H, MURRAY C B, O'BRIEN S P. Magnetic, electronic, and structural characterization of nonstoichiometric iron oxides at the nanoscale[J]. J Am Chem Soc, 2004, 126(44): 14583-14599.

    18. [18] WAN H J, WU B S, ZHANG C H, XIANG H W, LI Y W. Promotional effects of Cu and K on precipitated iron-based catalysts for Fischer-Tropsch synthesis[J]. J Mol Catal A: Chem, 2008, 283(1/2): 33-42.[18] WAN H J, WU B S, ZHANG C H, XIANG H W, LI Y W. Promotional effects of Cu and K on precipitated iron-based catalysts for Fischer-Tropsch synthesis[J]. J Mol Catal A: Chem, 2008, 283(1/2): 33-42.

    19. [19] 沈菊李, 刘化章, 李小年, 胡樟能, 国海光, 张天明. 费-托合成Fe1-xO基熔铁催化剂的研究[J]. 催化学报, 2004, 25(10): 785-788. (SHEN Ju-li, LIU Hua-zhang, LI Xiao-nian, HU Zhang-neng, GUO Hai-guang, ZHANG Tian-ming. Study on Fe1-xO-based fused iron catalyst for Fischer-Tropsch synthesis[J]. Chinese Journal of Catalysis, 2004, 25(10): 785-788.)[19] 沈菊李, 刘化章, 李小年, 胡樟能, 国海光, 张天明. 费-托合成Fe1-xO基熔铁催化剂的研究[J]. 催化学报, 2004, 25(10): 785-788. (SHEN Ju-li, LIU Hua-zhang, LI Xiao-nian, HU Zhang-neng, GUO Hai-guang, ZHANG Tian-ming. Study on Fe1-xO-based fused iron catalyst for Fischer-Tropsch synthesis[J]. Chinese Journal of Catalysis, 2004, 25(10): 785-788.)

  • 加载中
WeChat 扫一扫看文章
计量
  • PDF下载量:  0
  • 文章访问数:  696
  • HTML全文浏览量:  57
文章相关
  • 收稿日期:  2014-01-22
  • 网络出版日期:  2014-03-12
通讯作者: 陈斌, bchen63@163.com
  • 1. 

    沈阳化工大学材料科学与工程学院 沈阳 110142

  1. 本站搜索
  2. 百度学术搜索
  3. 万方数据库搜索
  4. CNKI搜索

/

返回文章

All Rights Reserved by the Chinese Chemical Society   中国化学会 版权所有 京ICP备05002797号

本系统由北京仁和汇智信息技术有限公司开发    技术支持: info@rhhz.net