SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2019, Vol. 27 ›› Issue (11): 2705-2711.DOI: 10.1016/j.cjche.2019.02.020

• Catalysis, Kinetics and Reaction Engineering • 上一篇    下一篇

Effect of sodium content on the interaction between Ni and support and catalytic performance for syngas methanation over Ni/Zr-Yb-O catalysts

Songshou Ye, Jiawei Guo, Yanbing Wang, Jianrong Xie, Zhiming Liu, Nuowei Zhang, Jinbao Zheng, Zhikai Cao, Binghui Chen   

  1. Department of Chemical and Biochemical Engineering, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
  • 收稿日期:2018-11-26 修回日期:2019-02-02 出版日期:2019-11-28 发布日期:2020-01-19
  • 通讯作者: Nuowei Zhang, Binghui Chen
  • 基金资助:
    Supported by the National Natural Science Foundation of China (21673187, 21336009, 21576228) and National Key Technology Support Program of China (2014BAC10B01).

Effect of sodium content on the interaction between Ni and support and catalytic performance for syngas methanation over Ni/Zr-Yb-O catalysts

Songshou Ye, Jiawei Guo, Yanbing Wang, Jianrong Xie, Zhiming Liu, Nuowei Zhang, Jinbao Zheng, Zhikai Cao, Binghui Chen   

  1. Department of Chemical and Biochemical Engineering, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
  • Received:2018-11-26 Revised:2019-02-02 Online:2019-11-28 Published:2020-01-19
  • Contact: Nuowei Zhang, Binghui Chen
  • Supported by:
    Supported by the National Natural Science Foundation of China (21673187, 21336009, 21576228) and National Key Technology Support Program of China (2014BAC10B01).

摘要: In this paper, Ni/Zr-Yb-O catalysts with different sodium contents are prepared by a co-precipitation method, using aqueous Na2CO3 solution as a precipitant, and the effect of sodium on the catalyst structure and catalytic performance for syngas methanation is extensively investigated using five Ni/Zr-Yb-O catalysts, containing 0, 0.5, 1.5, 4.5 and 13.5 wt% Na+, those are denoted as Cat-1, Cat-2, Cat-3, Cat-4 and Cat-5 respectively. It is found that the interaction between Ni and support determines the catalytic performance of Ni/Zr-Yb-O and the residual sodium content negatively affects the interaction between Ni and support. Cat-1 exhibits an excellent catalytic performance. During a long run time of 380 h, no deactivation is observed and both CO conversion and CH4 selectivity maintain a level above 90%. However, Cat-3 and Cat-5 suffer rapid deactivation under the same reaction condition. The characterization results indicate the strong interaction between Ni and support enables Cat-1 to possess well dispersed Ni species, resistance to sintering and carbon deposition and thus the excellent catalytic performance. However, the presence of sodium ions over Ni/Zr-Yb-O degrades the interaction between Ni and support and the catalytic performance, especially for the stability. The relative weak interaction between Ni and support results in severe sintering of both ZrO2 and Ni under the reaction condition, carbon deposition and the poor catalytic performance.

关键词: CO methanation, Ni/Zr-Yb-O catalyst, Sodium content, Syngas, Stability

Abstract: In this paper, Ni/Zr-Yb-O catalysts with different sodium contents are prepared by a co-precipitation method, using aqueous Na2CO3 solution as a precipitant, and the effect of sodium on the catalyst structure and catalytic performance for syngas methanation is extensively investigated using five Ni/Zr-Yb-O catalysts, containing 0, 0.5, 1.5, 4.5 and 13.5 wt% Na+, those are denoted as Cat-1, Cat-2, Cat-3, Cat-4 and Cat-5 respectively. It is found that the interaction between Ni and support determines the catalytic performance of Ni/Zr-Yb-O and the residual sodium content negatively affects the interaction between Ni and support. Cat-1 exhibits an excellent catalytic performance. During a long run time of 380 h, no deactivation is observed and both CO conversion and CH4 selectivity maintain a level above 90%. However, Cat-3 and Cat-5 suffer rapid deactivation under the same reaction condition. The characterization results indicate the strong interaction between Ni and support enables Cat-1 to possess well dispersed Ni species, resistance to sintering and carbon deposition and thus the excellent catalytic performance. However, the presence of sodium ions over Ni/Zr-Yb-O degrades the interaction between Ni and support and the catalytic performance, especially for the stability. The relative weak interaction between Ni and support results in severe sintering of both ZrO2 and Ni under the reaction condition, carbon deposition and the poor catalytic performance.

Key words: CO methanation, Ni/Zr-Yb-O catalyst, Sodium content, Syngas, Stability