NiZrO_(2)催化CO_(2)甲烷化机理模拟研究

RESEARCH ON THE MECHANISM OF CO_(2) METHANATION CATALYZED BY NiZrO_(2)

现有的ZrO_(2)负载Ni催化CO_(2)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CO_(2)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ZrO_(2)表面的吸附机理以及催化CO_(2)甲烷化过程的基元反应进行研究,阐明了NiZrO_(2)界面对CO_(2)的吸附、活化机制,明确了Ni、ZrO_(2)及其界面在CO_(2)加氢反应过程中的角色,提出了CO_(2)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。

The methanation of CO_(2) exhibits significant positive implications in multiple dimensions,including environmental protection,energy utilization and economic benefit enhancement.However,the intermediate species in the CO_(2) methanation process of ZrO_(2)-supported Ni catalyst are not clear,which hinders the development of new high efficient catalysts.The adsorption and activation mechanisms of CO_(2) at the Ni ZrO_(2) surface and the elementary reactions of the CO_(2) methanation process were studied by first-principles calculation,the roles of Ni,ZrO_(2) and their interface in the process of CO_(2) hydrogenation were clarified,and specific reaction paths in the process of CO_(2) methanation were proposed.This laid a solid foundation for the further development of efficient catalysts.