石油炼制与化工 ›› 2024, Vol. 55 ›› Issue (10): 41-47.

• 基础研究 • 上一篇    下一篇

Ni/ZrO2催化CO2甲烷化机理模拟研究

陈亚,曲亚坤,张荣俊,王丽新,赵晓光   

  1. 中石化石油化工科学研究院有限公司
  • 收稿日期:2024-03-13 修回日期:2024-06-03 出版日期:2024-10-12 发布日期:2024-09-26
  • 通讯作者: 陈亚 E-mail:chenya.ripp@sinopec.com
  • 基金资助:
    国家重点研发计划“政府间国际科技创新合作”重点专项

RESEARCH ON THE MECHANISM OF CO2 METHANATION CATALYZED BY Ni/ZrO2


  • Received:2024-03-13 Revised:2024-06-03 Online:2024-10-12 Published:2024-09-26

摘要: 现有的ZrO2负载Ni催化CO2甲烷化过程的中间物种不明晰,阻碍了新型高效催化剂的开发,限制了CO2甲烷化在环境保护、能源利用以及经济效益提升等多个层面的应用。通过第一性原理计算对Ni团簇在ZrO2表面的吸附机理以及催化CO2甲烷化过程的基元反应进行研究,阐明了Ni/ZrO2界面对CO2的吸附、活化机制,明确了Ni、ZrO2 及其界面在 CO2 加氢反应过程中的角色,提出了CO2甲烷化的具体反应路径,为高效催化剂的进一步开发奠定了坚实的基础。

关键词: Ni/ZrO2催化剂, 甲烷化, CO2利用, 第一性原理计算

Abstract: The methanation of CO2 exhibits significant positive implications in multiple dimensions, including environmental protection, energy utilization and economic benefit enhancement. However, the intermediate species in the CO2 methanation process of ZrO2-supported Ni catalyst are not clear, which hinders the development of new high efficient catalysts. The adsorption and activation mechanisms of CO2 at the Ni/ZrO2 surface and the elementary reactions of the CO2 methanation process were studied by first-principles calculation, the roles of Ni, ZrO2 and their interface in the process of CO2 hydrogenation were clarified, and specific reaction paths in the process of CO2 methanation were proposed. This laid a solid foundation for the further development of efficient catalysts.

Key words: Ni/ZrO2 catalyst, methanation, carbon dioxide utilization, first-principles calculations