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临CO2气氛下钼基催化剂耐硫甲烷化性能研究

李振花 ,  曲江磊 ,  王玮涵 ,  王保伟 ,  马新宾

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引用本文: 李振花, 曲江磊, 王玮涵, 王保伟, 马新宾. 临CO2气氛下钼基催化剂耐硫甲烷化性能研究[J]. 燃料化学学报, 2016, 44(08): 985-992. shu
Citation:  LI Zhen-hua, QU Jiang-lei, WANG Wei-han, WANG Bao-wei, MA Xin-bin. Effect of CO2 in syngas on methanation performance of Mo-based catalyst[J]. Journal of Fuel Chemistry and Technology, 2016, 44(08): 985-992. shu

临CO2气氛下钼基催化剂耐硫甲烷化性能研究

  • 1.

    天津大学化工学院 绿色合成与转化教育部重点实验室, 天津 300072

    • 通讯作者: 王玮涵
  • 基金项目:

    国家自然科学基金（21576203) 

    国家高技术研究发展计划（863计划，2015AA050504) 

    天津市应用基础与前沿技术研究计划重点项目（14JCZDJC37500）资助 

摘要: 在反应温度550℃、空速5000h-1和1.2% H2S浓度下，考察了反应气中添加CO2对负载型Mo基催化剂甲烷化活性的影响。结果表明，添加CO2会促进逆水煤气变换反应，从而降低MoO3/Al2O3催化剂的耐硫甲烷化活性。与MoO3/Al2O3催化剂相比，添加CO2对铈铝复合载体负载的Co-Mo双组分催化剂的影响较小。通过表征发现，添加CO2引起催化剂活性下降的主要原因是由于其增强了逆水煤气变换反应过程，使甲烷化过程可用氢气量减小。另外，逆水煤气变换反应生成的水会影响催化剂表面结构和组成。在连续加入10% CO2 20h后停止加入CO2，催化剂的耐硫甲烷化活性可以得到恢复，因此，认为CO2加入量低于10%时，对催化剂及甲烷化反应的影响是可逆的；但CO2加入量大于10%后由于生成的水量增大会破坏催化剂的结构并减少活性位，从而造成催化剂的不可逆失活。

English

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  • 收稿日期:  2016-02-29
  • 网络出版日期:  2016-04-23
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