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摘要: 通过原位引入Mg一步法合成了Mg@MCM-41复合介孔材料,并将其作为载体制备了高性能Ni基CO2甲烷化催化剂。通过BET、XRD、TEM、CO2-TPD、TG等手段对催化剂进行了表征分析,着重比较了Mg/Si物质的量比对于催化剂特性的影响。结果表明,当Mg/Si物质的量比为0.05时能够在不破坏孔道结构的前提下显著增加催化剂上的碱性位,有效地提高了催化剂对CO2的吸附和活化,从而促进CO2甲烷化反应过程中反应物的转化。实验所制得的催化剂均具有较好的热稳定性和催化反应活性,其中,Ni/0.05Mg@MCM-41在CO2甲烷化反应表现出最优的催化性能,在320 ℃,1 MPa的条件下,CO2转化率和CH4选择性分别高达84.3%和97.8%。Abstract: A series of xMg@MCM-41(x=0, 0.05, 0.1) functional mesoporous materials were synthesized by a novel in-situ one pot method and then were used as support for Ni based catalysts. The results of XRD and TEM show that when the amount of Mg/Si (molar ratio) is 0.05, Mg@MCM-4 with a regular and ordered mesoporous structure is synthesized where Mg is introduced into the framework of MCM-41. Introducing Mg into the framework of the support can significantly enhance the basic properties of the catalyst, thus promoting the adsorption and activation of CO2. The catalysts prepared in the experiments all have good thermal stability and catalytic activity. Among them, Ni/0.05Mg@MCM-41 shows the best low temperature reaction activity in the CO2 methanation reaction.
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Key words:
- CO2 /
- methanation /
- in-situ /
- Mg@MCM-41 /
- catalytic activity
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表 1 催化剂的物理化学特性
Table 1 Physicochemical properties of the catalysts
Catalyst ABET
/(m2·g-1)dpore/
nmvpore/
(cm3·g-1)Mg/Si
(molar ratio)Theoretical/% Actual w/% dNia/nm Mg Ni Mg Ni Ni/MCM-41 622.5 2.31 0.95 0 0 8.7 0.00 8.18 20 Ni/0.05Mg@MCM-41 606.3 3.37 0.84 0.05 1.78 8.7 1.94 8.28 15 Ni/0.1Mg@MCM-41 498.5 3.12 0.81 0.1 3.48 8.7 3.41 8.45 15 a: Ni size calculated by XRD -
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