杨丽, 宣国会, 刘方. 二氧化碳促进碳基化学链甲烷裂解制氢效率的实验和机理研究[J]. 中国电机工程学报, 2021, 41(18): 6321-6330. DOI: 10.13334/j.0258-8013.pcsee.201584
引用本文: 杨丽, 宣国会, 刘方. 二氧化碳促进碳基化学链甲烷裂解制氢效率的实验和机理研究[J]. 中国电机工程学报, 2021, 41(18): 6321-6330. DOI: 10.13334/j.0258-8013.pcsee.201584
YANG Li, XUAN Guohui, LIU Fang. Experiment and Mechanism of Carbon Dioxide on Promoting Chemical Looping Methane Decomposition Based on Activated Carbon Catalysts[J]. Proceedings of the CSEE, 2021, 41(18): 6321-6330. DOI: 10.13334/j.0258-8013.pcsee.201584
Citation: YANG Li, XUAN Guohui, LIU Fang. Experiment and Mechanism of Carbon Dioxide on Promoting Chemical Looping Methane Decomposition Based on Activated Carbon Catalysts[J]. Proceedings of the CSEE, 2021, 41(18): 6321-6330. DOI: 10.13334/j.0258-8013.pcsee.201584

二氧化碳促进碳基化学链甲烷裂解制氢效率的实验和机理研究

Experiment and Mechanism of Carbon Dioxide on Promoting Chemical Looping Methane Decomposition Based on Activated Carbon Catalysts

  • 摘要: 天然气中所含的少量CO2杂质会影响化学链甲烷裂解制氢效率。以8~16目椰壳活性炭为多功能载体,研究在850,900℃和950℃温度下0~7.2%的CO2对甲烷裂解效率的影响。结果表明,不同浓度的CO2可以提高甲烷裂解效率,其中4.8%的CO2浓度最有利。对CO2促进甲烷裂解效率机理的进一步研究表明,CO2的促进作用主要表现在反应前期阶段。研究还表明,CO2难以与积碳反应,消碳作用并不明显。采用Materials Studio软件模拟了高温下CO2对活性炭表面甲烷分子吸附的影响,结果表明CO2对吸附过程没有明显影响。进一步表征和分析表明,尽管加入CO2不会改变活性炭含氧官能团的类型,但可有效提高含氧官能团浓度,这有利于增加活性位点,从而改善活性炭的催化性能。

     

    Abstract: Small amounts of CO2 impurities contained in natural gas affect the efficiency of chemical looping methane decomposition for hydrogen production. 8-16 mesh coconut shell activated carbon (AC) was used as a multifunctional carrier, and the effect of 0-7.2% CO2 on methane decomposition efficiency was studied at temperatures of 850, 900℃ and 950℃. The results show that CO2 at different concentrations could improve the decomposition efficiency of methane, among which the 4.8% CO2 concentration was the most favorable. Further studies on the mechanism of CO2 in promoting the efficiency of methane decomposition revealed that positive impact of CO2 was mainly manifested in the early stage of AC. Studies also showed that CO2 was difficult to react with deposited carbon, and its role in deposited carbon elimination was not obvious. Materials Studio software was used to simulate the effect of CO2 on the adsorption of methane molecules on AC at high temperatures, and the results showed that CO2 had no significant effect on the adsorption process. Further characterization and analysis showed that although the addition of CO2 did not change the type of oxygen-containing functional groups, it could effectively increase the concentration of oxygen-containing functional groups, which was beneficial to the increase in active sites, thereby improving the catalytic performance of AC

     

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