化工进展 ›› 2021, Vol. 40 ›› Issue (12): 6925-6933.DOI: 10.16085/j.issn.1000-6613.2020-2553

• 资源与环境化工 • 上一篇    下一篇

碱/碱土金属修饰Ni基催化剂的CO2吸附与甲烷化性能

王国栋(), 郭亚飞(), 李佳媛, 姚睿璇, 孙健, 赵传文()   

  1. 南京师范大学能源与机械工程学院,江苏 南京 210046
  • 收稿日期:2020-12-23 修回日期:2021-03-06 出版日期:2021-12-05 发布日期:2021-12-21
  • 通讯作者: 郭亚飞,赵传文
  • 作者简介:王国栋(1995—),男,硕士研究生,研究方向为CO2捕集与转化利用。E-mail:1041890465@qq.com
  • 基金资助:
    国家自然科学基金(51806108);能源清洁利用国家重点实验室开放基金(ZJUCEU2020009);江苏省研究生科研创新项目(KYCX21-1379)

CO2 adsorption and methanation performance of nickel-based catalysts modified with alkali/alkaline-earth metals

WANG Guodong(), GUO Yafei(), LI Jiayuan, YAO Ruixuan, SUN Jian, ZHAO Chuanwen()   

  1. School of Energy and Mechanical Engineering, Nanjing Normal University, Nanjing 210046, Jiangsu, China
  • Received:2020-12-23 Revised:2021-03-06 Online:2021-12-05 Published:2021-12-21
  • Contact: GUO Yafei,ZHAO Chuanwen

摘要:

采用分步浸渍法制备了碱/碱土金属修饰Ni基催化剂Ni-M/Al2O3 (M=K2CO3, Na2CO3, MgO, CaO)。探究了碱/碱土金属的添加对改性Ni基催化剂CO2吸附和甲烷化性能的影响。研究发现,碱/碱土金属的添加提高了Ni/Al2O3催化剂表面的碱性活性位点密度,强化了其CO2吸附性能。碱/碱土金属类型影响Ni-M/Al2O3催化剂碱性活性位点的分布、NiO物相的转化及Ni的分散度,进而影响其甲烷化性能。MgO添加使NiO物相转化为与载体呈强相互作用的β型和γ型NiO,降低了催化剂表面的强碱性活性位点比例,有利于CO2吸附活化。Ni-MgO/Al2O3的CO2吸附容量最高为0.68mmolCO2/g,其CO2转化率和CH4选择性分别高达58.4%和95.4%,其在烟气CO2捕集与原位甲烷化中极具应用前景。

关键词: 碱/碱土金属, 催化剂, CO2捕集, 加氢, 甲烷化, 选择性

Abstract:

A series of nickel-based catalysts modified with alkali/alkaline-earth metals (Ni-M/Al2O3, M= K2CO3, Na2CO3, MgO, CaO) were prepared by step impregnation method. Effects of the doped alkali/alkaline-earth metals on CO2 adsorption and methanation performance of the modified Ni-M/Al2O3 catalysts were investigated. Doping alkali/alkaline-earth metals increased the surface density of basic active sites of Ni/Al2O3 catalyst and therefore enhanced the CO2 adsorption capacity. The doped alkali/alkaline-earth metals could also affect the distribution of the surface basic active sites, the transformation of NiO phase and the dispersion of Ni on the support, and therefore the Ni-M/Al2O3 catalysts exhibited different methanation performance. MgO doping would promote the transformation of NiO to β- and γ-type NiO phases, which exhibited strong interaction with the support. Besides, MgO doping reduced the proportion of strong basic active sites, which could be favorable for CO2 adsorption and activation. Amongst the Ni-M/Al2O3 catalysts, Ni-MgO/Al2O3 exhibited the highest CO2 adsorption capacity of 0.68 mmol CO2/g, the maximum CO2 conversion of 58.4% and the greatest CH4 selectivity of 95.4%. The Ni-MgO/Al2O3 catalyst showed potential application in CO2 capture from flue gas and in-situ methanation.

Key words: alkali/alkaline-earth metals, catalysts, CO2 capture, hydrogenation, CO2 methanation, selectivity

中图分类号: 

京ICP备12046843号-2;京公网安备 11010102001994号
版权所有 © 《化工进展》编辑部
地址:北京市东城区青年湖南街13号 邮编:100011
电子信箱:hgjz@cip.com.cn
本系统由北京玛格泰克科技发展有限公司设计开发 技术支持:support@magtech.com.cn