化工进展 ›› 2023, Vol. 42 ›› Issue (5): 2421-2428.DOI: 10.16085/j.issn.1000-6613.2022-1260

• 工业催化 • 上一篇    下一篇

CeO2-Al2O3复合载体负载Ni基催化剂催化CO x 共甲烷化性能

马源1,2(), 肖晴月1,3, 岳君容1, 崔彦斌1, 刘姣1(), 许光文3   

  1. 1.中国科学院过程工程研究所多相复杂系统国家重点实验室,北京 100190
    2.中南大学化学化工学院,湖南 长沙 410083
    3.沈阳化工大学能源与化工产业技术研究院,辽宁 沈阳 110142
  • 收稿日期:2022-07-05 修回日期:2022-10-15 出版日期:2023-05-10 发布日期:2023-06-02
  • 通讯作者: 刘姣
  • 作者简介:马源(1995—),女,博士研究生,研究方向为纳米材料的制备与表征。E-mail:mayuan95mvp@163.com
  • 基金资助:
    国家重点研发计划(2019YFC1906802)

CO xco-methanation over a Ni-based catalyst supported on CeO2-Al2O3 composite

MA Yuan1,2(), XIAO Qingyue1,3, YUE Junrong1, CUI Yanbin1, LIU Jiao1(), XU Guangwen3   

  1. 1.State Key Laboratory of Muti-Phase Complex System, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
    2.College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, Hunan, China
    3.Institute of Industrial Chemistry and Energy Technology, Shenyang University of Chemical Technology, Shenyang 110142, Liaoning, China
  • Received:2022-07-05 Revised:2022-10-15 Online:2023-05-10 Published:2023-06-02
  • Contact: LIU Jiao

摘要:

通过浸渍沉淀法分别制备Ni/Al2O3、Ni/CeO2和Ni/CeO2-Al2O3催化剂,并对其分别进行不同CO/CO2比例下CO x 共甲烷化性能评价。发现Ni/Al2O3催化剂催化CO转化为CH4的能力明显高于Ni/CeO2,而催化CO2甲烷化的性能则相反。采用Ni/CeO2-Al2O3催化剂,可以在提高CO转化率的同时而不降低CO2转化率。结合BET、XRD、TPR、TPD和原位红外等各种表征手段,发现CeO2掺杂虽然降低了催化剂的比表面积和金属Ni的分散度,但却可明显提高其吸附活化CO2的能力,这主要是由于具有较高含量氧空位的CeO2的掺杂可以提高载体表面碱性位,促使共甲烷过程中CO2吸附活化并形成单齿碳酸盐,通过快速加氢反应生成目标产物甲烷;而Ni/Al2O3受限于其对CO2的吸附容量和活化产物双齿碳酸盐的活性,在催化共甲烷化体系中只能获得较低的CO2转化率,但CO转化率不受影响。

关键词: 二氧化碳, 一氧化碳, 甲烷化, 催化剂载体, 镍, 碱性位

Abstract:

Ni/Al2O3, Ni/CeO2 and Ni/CeO2-Al2O3 catalysts were prepared by impregnation-precipitation method and applied for CO xco-methanation with different ratios of CO/CO2. It was found that the conversion of CO to CH4 was higher over Ni/Al2O3 than thatover Ni/CeO2, while CO2 methanation gave reverse order. Adopting Ni/CeO2-Al2O3 as CO xco-methanation catalyst improved the CO conversion without lessening CO2 conversion. BET, XRD, TPR, TPD and in-situ FTIR characterizations showed that the surface area and dispersion degree of metallic nickel decreased after CeO2 was dopped in Al2O3. However, the CO2 adsorption and activation capacity were increased, because the rich oxygen vacancies on CeO2 would increase the basic sites on the support which activated CO2 to monodentate carbonate, and then be hydrogenated to methane quickly. Limited by the CO2 adsorption capacity and the activity of the medium product-bidentate carbonate, the CO2 conversion over Ni/Al2O3 catalyst was lower than that over Ni/CeO2-Al2O3 catalyst while CO conversion was unaffected during CO xco-methanation.

Key words: carbon dioxide, carbon monoxide, methanation, catalyst support, nickel (Ni), basic site

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