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摘要: 针对CH4在熔融碳酸盐中转化的新体系，研究了CH4在熔融碳酸盐介质中的还原行为。对CH4与熔融碳酸盐(Li2CO3、Na2CO3、K2CO3)的反应产物组分作了热力学分析，进行了实验研究，并对反应机制进行了探讨。研究结果表明，气体产物中CO、CO2的含量随反应温度的升高而增加；随反应时间的增加而降低；反应活性大小变化规律为：Li2CO3>Na2CO3 >K2CO3，实验结果与理论分析相符。混合熔融盐具有更高的CO选择性，并且气体产物中CO、CO2浓度及CH4转化率随反应时间增加降低较快，较纯组分更适合作CH4转化反应介质。反应机制的推测表明H2、CO、CO2的产生分别来自于CH4裂解及裂解C与熔融碱金属碳酸盐的反应。Abstract: The methane reduction behavior was studied in a molten alkali carbonates (Li2CO3、Na2CO3、K2CO3) system. Thermodynamic and experimental investigations were performed to quantify the product compositions. The results showed that the CO and CO2 contents in the product gases increased with the reaction temperature, whereas it decreased with the reaction time. The reaction activity order of carbonates was Li2CO3 > Na2CO3 > K2CO3. The selectivity of CO in the mixed molten salts system was higher than that in a pure system. The mixed molten salts system was more suitable than pure system as the reaction medium of CH4 conversion. H2 was mainly from the CH4 cracking, and CO and CO2 was from the reaction between CH4 cracking carbon and molten alkali carbonates.
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Key words:
- methane /
- molten alkali carbonate /
- reduction behavior /
- thermodynamic analysis /
- reaction mechanism
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