Reaction Kinetics, Mechanisms and Catalysis ( IF 1.7 ) Pub Date : 2023-02-24 , DOI: 10.1007/s11144-023-02377-0 Zhanggui Hou , Yiming Chen , Chuan Wang , Xin Ma , Hong Yang , Wen Wang , Yi Zhang
The Mn promoted Ni catalysts were developed and applied in CO methanation reaction. The 10%Ni/SiO2 catalyst exhibits poor initial CO conversion (32.8%) and rapid deactivation with the highest methane selectivity during CO methanation reaction. In contrast, the Mn 4%Mn-10%Ni/SiO2 catalyst shows dramatically increased initial CO conversion, which is up to 94.5% with 90.0% methane selectivity. Besides, the apparent activation energy, Ea value, of 4%Mn-10%Ni/SiO2 was calculated to be 73.1 kJ/mol according to Arrhenius equation, which is much lower than that of 10%Ni/SiO2 catalyst as 139.1 kJ/mol. Based on various characterization results, including in situ XPS and in situ CO-DRIFTS, it is found that the added Mn significantly improves the dispersion of the supported nickel, suppresses the sintering of nickel particles and forms more adsorbed CO species of three-fold carbonyl species, resulting in higher CO conversion and good stability during CO methanation reaction.
中文翻译:
Mn对Ni/SiO2催化剂CO甲烷化的促进作用
开发了Mn助催化的Ni催化剂并将其应用于CO甲烷化反应。10%Ni/SiO 2催化剂表现出较差的初始 CO 转化率 (32.8%) 和在 CO 甲烷化反应期间具有最高甲烷选择性的快速失活。相比之下,Mn 4%Mn-10%Ni/SiO 2催化剂显示初始 CO 转化率显着增加,高达 94.5%,甲烷选择性为 90.0%。此外,根据Arrhenius方程计算出4%Mn-10%Ni/SiO 2的表观活化能Ea值为73.1 kJ/mol,远低于10%Ni/SiO 2的表观活化能Ea值。催化剂为 139.1 kJ/mol。基于各种表征结果,包括原位 XPS 和原位 CO-DRIFTS,发现添加的 Mn 显着改善了负载镍的分散性,抑制了镍颗粒的烧结并形成了更多吸附的三重羰基 CO 物种种,从而在 CO 甲烷化反应过程中产生更高的 CO 转化率和良好的稳定性。