物理化学学报 >> 2008, Vol. 24 >> Issue (09): 1568-1572.doi: 10.3866/PKU.WHXB20080907

研究论文 上一篇    下一篇

La2O3对沼气重整制氢催化剂Ni/γ-Al2O3的影响

徐军科; 任克威; 王晓蕾; 周伟; 潘相敏; 马建新   

  1. 同济大学环境科学与工程学院, 上海 200092; 同济大学新能源汽车工程中心, 上海 201804; 华东理工大学资源与环境工程学院,上海 200237
  • 收稿日期:2008-03-26 修回日期:2008-05-11 发布日期:2008-09-10
  • 通讯作者: 马建新 E-mail:jxma@mail.tongji.edu.cn

Effect of La2O3 on Ni/γ-Al2O3 Catalyst for Biogas Reforming to Hydrogen

XU Jun-Ke; REN Ke-Wei; WANG Xiao-Lei; ZHOU Wei; PAN Xiang-Min; MA Jian-Xin   

  1. School of Environmental Science and Engineering, Tongji University, Shanghai 200092, P. R. China; Clean Energy Automotive Engineering Center, Tongji University, Shanghai 201804, P. R. China; School of Resource and Environmental Engineering, East China University of Science and Technology, Shanghai 200237, P. R. China
  • Received:2008-03-26 Revised:2008-05-11 Published:2008-09-10
  • Contact: MA Jian-Xin E-mail:jxma@mail.tongji.edu.cn

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摘要： 用浸渍法制备了不同La2O3含量的Ni/La2O3/γ-Al2O3催化剂, 用CH4/CO2体积比为1的混合气体模拟沼气, 考察了La2O3对沼气重整制氢催化剂Ni/γ-Al2O3的结构及催化性能的影响. 运用XRD、H2-TPR、BET及TEM等手段对催化剂进行了表征. 结果表明, La2O3对催化剂Ni/γ-Al2O3的影响主要取决于其含量. 载体中La2O3的添加增强了Ni与Al2O3之间的相互作用. 添加适量的La2O3能使催化剂具有更好的可还原性, 并能增加金属Ni的分散性, 抑制反应过程中Ni的烧结, 提高载体对CO2的吸附能力, 从而改善了催化剂的抗积炭性, 使催化剂具有较好的活性及稳定性. 反之, 过量La2O3的掺杂会使催化剂的抗积炭性及活性下降. 当La2O3含量为6%(w)时, 催化剂中Ni晶粒具有较好的分散性、还原性及抗积炭性, 从而使催化剂具有更好的活性及稳定性.

关键词: 氧化镧, 镍, 氧化铝, 沼气重整, 制氢, 分散性, 抗积炭性

Abstract: Ni/γ-Al2O3 catalysts modified by La2O3 were prepared with incipient wetness impregnation and used in biogas reforming to hydrogen. The catalysts were characterized with XRD, H2-TPR, BET, and TEM, respectively, and the relationship between the performance and the structural properties of the catalysts was investigated. The biogas was simulated with CH4 and CO2, and the volume ratio of CH4/CO2 was 1. The results showed that the amount of La2O3 added was a key influence factor. The increment of La2O3 in γ-Al2O3 support strengthened the interaction between Ni and γ-Al2O3. Appropriate accession of La2O3 could improve the reducibility of catalysts, increase the dispersity of metallic Ni on support, suppress the sintering of metallic Ni particles and enhance the adsorption of CO2 on support during the reaction. As a result, the performance of catalyst, including resistance to coking, activity and stability, was improved significantly. However, excessive addition of La2O3 deteriorated the performance of catalyst. It was found that the best performance of catalyst could be reached at the addition of 6% (w) La2O3 in γ-Al2O3.

Key words: Lanthanumoxide, Nickel, Alumina, Biogas reforming, Hydrogen production, Dispersity, Resistance to coking