改性铝土矿载体负载Ru催化剂上的水煤气变换制氢

doi:10.3866/PKU.WHXB201112271

物理化学学报 >> 2012, Vol. 28 >> Issue (03): 674-680.doi: 10.3866/PKU.WHXB201112271

改性铝土矿载体负载Ru催化剂上的水煤气变换制氢

江莉龙, 马永德, 曹彦宁, 杨阳, 魏可镁

福州大学化肥催化剂国家工程研究中心, 福州 350002

收稿日期:2011-09-19 修回日期:2011-12-19 发布日期:2012-02-23
通讯作者: 江莉龙 E-mail:jll@fzu.edu.cn
基金资助:
福建省自然科学基金(2011J01036), 福建省教育厅基金(JA09012), 福州大学人才启动基金及福州大学科技发展基金项目(2010-XQ-05)资助

Modified Bauxite Supported Ruthenium Catalysts for Hydrogen Evolution in the Water-Gas Shift Reaction

JIANG Li-Long, MA Yong-De, CAO Yan-Ning, YANG Yang, WEI Ke-Mei

National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, P. R. China

Received:2011-09-19 Revised:2011-12-19 Published:2012-02-23
Contact: JIANG Li-Long E-mail:jll@fzu.edu.cn
Supported by:
The project was supported by the Natural Science Foundation of Fujian Province, China (2011J01036), Foundation of Fujian Provincial Department of Education, China (JA09012), Talents Foundation of Fuzhou University, China, and Technology Development Foundation of Fuzhou University, China (2010-XQ-05).

摘要/Abstract

摘要： 采用水热法对天然铝土矿进行改性, 获得高比表面积的铝土矿(bauxite)载体. 用等体积浸渍法制备了Ru含量为1.0%-4.0%(质量分数, 下同)的Ru/bauxite 催化剂和Ru含量为2.0%的Ru/Al₂O₃催化剂, 以水煤气变换反应为探针反应, 考察了催化剂性能. 利用X射线荧光元素分析(XRF)、X射线粉末衍射(XRD)、低温N₂物理吸附、H₂程序升温还原(H₂-TPR)以及CO程序升温脱附(CO-TPD)等对载体和催化剂样品进行表征. 结果表明, 不同Ru含量的Ru/bauxite 催化剂具有优异的水煤气变换制氢性能, 优于Ru/Al₂O₃催化剂. 其原因是铝土矿本身含有的Fe₂O₃与负载的Ru之间发生了相互作用, 降低了Fe₂O₃还原温度, 提高了对CO的吸附能力且降低了CO的脱附温度, 进而提高了催化剂的水煤气变换反应性能.

关键词: 铝土矿, Ru/铝土矿催化剂, 水煤气变换, 制氢

Abstract: Hydrothermally treated bauxite with high surface area was used as a ruthenium-based catalyst support. A series of Ru/bauxite and 2.0% (mass fraction) Ru/Al₂O₃ catalysts were prepared by incipientwetness impregnation. The loading content of ruthenium in the Ru/bauxite catalysts was varied from 1.0% to 4.0%. The catalysts were thoroughly characterized by X-ray fluorescence (XRF), low temperature N₂ physical adsorption, X-ray diffraction (XRD), H₂ temperature-programmed reduction (H₂-TPR), and CO temperature-programmed desorption (CO-TPD). The performances of the catalysts for the water-gas shift reaction were also investigated. The results indicated that Ru/bauxite catalysts possess an excellent ability to evolve hydrogen in the water-gas shift reaction. This was attributed to the interaction between Ru and Fe₂O₃ in the modified bauxite, which could decrease the reduction temperature of Fe₂O₃, and also improve the adsorption-desorption behavior and decrease the desorption temperature of Ru/bauxite catalysts for CO molecules, resulting in higher activity in the water-gas shift reaction.

Key words: Bauxite, Ru/bauxite catalyst, Water-gas shift, Hydrogen evolution

MSC2000:

O643

江莉龙, 马永德, 曹彦宁, 杨阳, 魏可镁. 改性铝土矿载体负载Ru催化剂上的水煤气变换制氢[J]. 物理化学学报, 2012, 28(03): 674-680.

JIANG Li-Long, MA Yong-De, CAO Yan-Ning, YANG Yang, WEI Ke-Mei. Modified Bauxite Supported Ruthenium Catalysts for Hydrogen Evolution in the Water-Gas Shift Reaction[J]. Acta Phys. -Chim. Sin., 2012, 28(03): 674-680.

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改性铝土矿载体负载Ru催化剂上的水煤气变换制氢

Modified Bauxite Supported Ruthenium Catalysts for Hydrogen Evolution in the Water-Gas Shift Reaction

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