浆态床镍基甲烷化催化剂的研究
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摘要
浆态床反应器具有传热迅速,热稳定性高等特点,将浆态床反应器引入甲烷化过程中,可以克服催化剂因高温烧结而造成的失活问题,保持系统的稳定性。本文制备了以二氧化硅为载体的镍基浆态床甲烷化催化剂,优化了制备条件：在450-550℃焙烧,550℃还原时活性组分分散均匀,催化剂催化效果较好；Y-AI2O3形态的铝助剂可以有效的提高催化剂的选择性,而助剂在没有硫元素的情况抑制了催化效果；稀土元素镧和铈不仅提高了CO转化率而且对甲烷的选择性也较好。采用商用催化剂和制备的镍基催化剂,在浆态床反应器上进行了单因素优化,优化结果为：反应温度为290℃C-300℃,原料气中H2/CO的比例为3：1和3.5：1时。压力对摧化剂影响不明显,空速增大提高了反应速率,同时也降低了催化剂的单程转化率。
There are some advantages for the slurry bed reactor:high heat-transfer coefficient, high stability and so on. The catalysts sintering and losing activity could be reduced or avoided by using the slurry bed reactor in methanation production. And the process of reactor was well stability. The catalyst of nickel based on silica for methanation in slurry bed reactor was prepared in this paper. The results show that the catalyst calcinated at among450-550℃and reduced at550℃could improve nickel distribution on support and catalytic activity. The γ-Al2O3is very well promoter in methanation catalyst, and it could increase the selectivity of methane. The promoter research also showed that rare-earth element improved the CO conversion and the selectivity of methane, and Mo promoter reduced the catalytic results without sulfur. The process conditions of the catalyst were also studied, and the optimized conditions are that, the reaction temperature was at290℃or300℃, H2/CO were equal to3:1or3.5:1. The pressure had little effect, and2MPa was used in the paper. High gas-speed could reduce the CO conversion per pass and increase the reaction rate.
There are some advantages for the slurry bed reactor:high heat-transfer coefficient, high stability and so on. The catalysts sintering and losing activity could be reduced or avoided by using the slurry bed reactor in methanation production. And the process of reactor was well stability. The catalyst of nickel based on silica for methanation in slurry bed reactor was prepared in this paper. The results show that the catalyst calcinated at among450-550℃and reduced at550℃could improve nickel distribution on support and catalytic activity. The γ-Al2O3is very well promoter in methanation catalyst, and it could increase the selectivity of methane. The promoter research also showed that rare-earth element improved the CO conversion and the selectivity of methane, and Mo promoter reduced the catalytic results without sulfur. The process conditions of the catalyst were also studied, and the optimized conditions are that, the reaction temperature was at290℃or300℃, H2/CO were equal to3:1or3.5:1. The pressure had little effect, and2MPa was used in the paper. High gas-speed could reduce the CO conversion per pass and increase the reaction rate.
引文
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