| 张颜鑫,张因,赵永祥.ZrO2晶型对Ni/ZrO2催化剂CO甲烷化性能的影响[J].分子催化,2013,(4):349-355 |
| ZrO2晶型对Ni/ZrO2催化剂CO甲烷化性能的影响 |
| Effect of ZrO2 Polymorphs on Catalytic Performance of Ni/ZrO2 Catalysts for CO Methanation |
| 投稿时间：2013-04-22 修订日期：2013-06-17 |
| DOI： |
| 中文关键词: m-ZrO2 t-ZrO2 Ni基催化剂 CO甲烷化 |
| 英文关键词:m-ZrO2 t-ZrO2 Nickel-based catalyst ZrO2 polymorph CO methanation |
| 基金项目:山西省“十二五”科技重大专项(20111101010)，国际科技合作专项(2013DFA40460) |
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| 中文摘要: |
| 采用浸渍法制备了四方相ZrO2(t-ZrO2)和单斜相ZrO2(m-ZrO2)负载的Ni含量为10 wt%的催化剂，在连续流动微反装置上考察了Ni/m-ZrO2以及不同温度焙烧Ni/t-ZrO2催化剂的CO甲烷化催化活性。采用N2物理吸附-脱附、H2-TPR、XRD、CO-TPSR及原位漫反射傅里叶变换红外光谱等技术对催化剂进行了表征。结果表明，在CO体积分数为1%，空速为20000 h-1，常压的反应条件下，当CO转化率为50%时，Ni/m-ZrO2-673和Ni/t-ZrO2-673催化剂的反应温度分别为445 K和488 K，Ni/m-ZrO2-673催化剂的CO甲烷化活性远高于Ni/t-ZrO2-673催化剂。随焙烧温度的升高，Ni/t-ZrO2催化剂的CO甲烷化活性评价显著升高，产生这一现象的原因是在高温焙烧过程中Ni/t-ZrO2催化剂表面的t-ZrO2已转化为m-ZrO2，以m-ZrO2为载体的催化剂因m-ZrO2表面具有较多的配位不饱和O2-碱性中心和配位不饱和Zr4+-O2-位点而表现出高的CO甲烷化活性。 |
| 英文摘要: |
| The catalytic activities for CO methanation of the Ni/m-ZrO2 catalyst and Ni/t-ZrO2 catalysts calcined at different temperatures were investigated by a continuous flowing microreactor apparatus. All the catalysts were characterized by N2 physical adsorption-desorption, H2-TPR, XRD, CO-TPSR and In-situ DRIFTS. Under the reaction conditions: CO 1%、GHSV 5000 h-1 and an atmosphere pressure, the T50% temperature for Ni/m-ZrO2-673 and Ni/t-ZrO2-673 catalyst was 445 K and 488 K, respectively. The catalytic activity for CO methanation of Ni/m-ZrO2-673 catalyst is much higher than that of the Ni/t-ZrO2-673 catalyst. As the calcination temperature increased, the catalytic activity of Ni/t-ZrO2 catalyst was significantly increased. Further characterization demonstrated that the reason for this phenomenon resided that the surface t-ZrO2 of Ni/t-ZrO2 catalyst convert to m-ZrO2 during the heat treatment. Due to m-ZrO2 has more unsaturated coordinatively O2- basic centers and coordinated unsaturated Zr4+-O2- acid-base centers, Ni/m-ZrO2 catalyst exhibited higher catalytic activity for CO methanation. |
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