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Enhanced performance and selectivity of CO2 methanation over phyllosilicate structure derived Ni-Mg/SBA-15 catalysts
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-09-20 , DOI: 10.1016/j.apcatb.2020.119564
Plaifa Hongmanorom , Jangam Ashok , Guanghui Zhang , Zhoufeng Bian , Ming Hui Wai , Yiqing Zeng , Shibo Xi , Armando Borgna , Sibudjing Kawi

Ni and Ni-Mg phyllosilicate mesoporous SBA-15 catalysts were successfully prepared via ammonia evaporation (AE) method as evidenced by XRD, H2-TPR, TEM, FTIR and EXAFS fitting results. The catalysts derived from phyllosilicate structure exhibit superior catalytic performance in CO2 methanation as compared to catalyst prepared via wetness impregnation (WI) method due to enhanced metal-support interaction and the presence of weakly basic sites provided by surface hydroxyl groups. Incorporation of Mg into phyllosilicate structure with optimum 5 wt% is also found to increase medium basic sites, which can promote monodentate formate formation as identified by DRIFTS analysis and improve CO2 methanation activity at lower temperatures. Additionally, the turnover frequency of CO2 conversion can be well correlated with the concentration of basic sites. The strong metal-support interaction derived from phyllosilicate structure along with confinement effect of SBA-15 can suppress metal sintering, resulting in good stability.



中文翻译:

在页硅酸盐结构衍生的Ni-Mg / SBA-15催化剂上提高了CO 2甲烷化的性能和选择性

XRD,H 2 -TPR,TEM,FTIR和EXAFS拟合结果证明,通过氨蒸发(AE)方法成功制备了Ni和Ni-Mg页硅酸盐介孔SBA-15催化剂。与通过湿法浸渍(WI)方法制备的催化剂相比,源自页硅酸盐结构的催化剂在CO 2甲烷化中表现出优异的催化性能,这归因于增强的金属-载体相互作用以及表面羟基提供的弱碱性位点的存在。还发现以最佳的5 wt%将Mg掺入页硅酸盐结构中可以增加中等的碱性位点,如DRIFTS分析所确定的,这可以促进单齿甲酸盐的形成并改善CO 2低温下的甲烷化活性。另外,CO 2转化的周转频率可以与碱性位点的浓度很好地相关。源于页硅酸盐结构的强金属-载体相互作用以及SBA-15的限制作用可以抑制金属烧结,从而具有良好的稳定性。

更新日期:2020-10-08
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