CIESC Journal ›› 2022, Vol. 73 ›› Issue (1): 241-254.DOI: 10.11949/0438-1157.20210778

• Catalysis, kinetics and reactors • Previous Articles     Next Articles

Research on promotion of Fe in Ni/SBA-16 catalyzing CO methanation at low temperature

Wenli GAO1(),Zhong XIN1,2()   

  1. 1.Shanghai Key Laboratory of Multiphase Materials Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
    2.State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
  • Received:2021-06-09 Revised:2021-09-14 Online:2022-01-18 Published:2022-01-05
  • Contact: Zhong XIN

Fe对Ni/SBA-16催化CO低温甲烷化促进作用的研究

高文莉1(),辛忠1,2()   

  1. 1.华东理工大学化工学院,上海市多相结构材料化学工程重点实验室,上海 200237
    2.华东理工大学,化学工程联合国家重点实验室,上海 200237
  • 通讯作者: 辛忠
  • 作者简介:高文莉(1992—),女,博士研究生,double719917@126.com
  • 基金资助:
    国家自然科学基金项目(21808062);中央高校基本科研业务费专项资金项目(22A1817025);上海市双一流配套专项

Abstract:

To improve the activity of Ni/SBA-16 catalyst in CO methanation at low temperature, Ni-Fe/SBA-16 bimetallic catalyst was prepared by introducing Fe promoter. The results of XPS, XRD, HRTEM and EDS-mapping characterization of the catalyst show that the addition of Fe forms a Ni3Fe alloy with Ni, which reduces the size of the metal particles and reduces the average particle size of the metal particles from 60 nm to about 30 nm after reduction. Meanwhile, the H2-TPR results showed that the formation of Ni3Fe alloy strengthened the metal-support interaction, which would weaken the agglomeration of metal particles during the process of reduction and reaction. Finally, the analysis of CO-TPD and H2-TPD indicated that the formation of Ni3Fe alloy promoted the dissociation of reactant gas (CO and H2), thus enhancing the catalytic activity of CO methanation catalyst at low temperature. As a result, the CO minimum complete conversion temperature was lowered to 250°C from 300°C with a CH4 selectivity of 90% eventually at the condition of space velocity 150000 h-1, P=0.1 MPa, V(H2)∶V(CO)∶V(N2)=3∶1∶1.

Key words: bimetalliccatalysts, carbon monoxide, methane, mesoscale, molecular sieves, nanoparticles

摘要:

为了提高Ni/SBA-16催化剂在低温下CO甲烷化中的活性,通过引入Fe助剂制备了Ni-Fe/SBA-16双金属催化剂。对催化剂进行XPS、XRD、HRTEM及EDS-mapping表征的结果表明,Fe的加入与Ni形成了Ni3Fe合金,减小了金属颗粒尺寸,使得还原后金属颗粒平均粒径从60 nm降低到30 nm左右。同时H2-TPR的结果表明,Ni3Fe合金的形成增强了金属Ni与载体之间的相互作用,从而能够减弱Ni颗粒在还原过程及反应过程中的团聚。最后,由CO-TPD和H2-TPD的测试结果可知,Ni3Fe合金的形成促进了催化剂对反应气体CO和H2的解离,从而提高了催化剂在低温下的CO甲烷化活性。当空速为150000 h-1、压力为0.1 MPa、V(H2)∶V(CO)∶V(N2)=3∶1∶1时,CO最低完全转化温度可以从300°C降低到250°C,同时CH4的选择性保持在90%。

关键词: 双金属催化剂, 一氧化碳, 甲烷, 介尺度, 分子筛, 纳米颗粒

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