CO2甲烷化的现场监测:在CO2和H2条件下球磨LaNi5的压力变化

Keito Sawahara, Ryota Gemma
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引用次数: 1

摘要

近年来,大气中二氧化碳浓度迅速增加,可能加剧持续的全球变暖问题。这里,大气中二氧化碳的甲烷化已经被提出。然而,在目前开发的甲烷化过程中,使用镍等催化剂至少需要200-300°C。因此,从节能的角度出发,通过不同的工艺降低反应温度,避免催化剂在高温下失活是可取的。我们最近报道了La-Ni基合金在CO2和H2存在下的机械化学过程成功地生成了CH4。但是,本研究的原子探针断层扫描(APT)分析也表明,在球磨过程中,CO2可能与LaNi5粉末发生了部分反应,生成了不同的La-氧化物、羧化物和含有La嵌入Ni基体的羟基物质。这些化合物可能是甲烷化反应的有效中间相。为了阐明催化活性的来源,有必要对过程中的压力变化进行现场监测;在上述过程中,还应研究CO2与LaNi5的反应性。介绍了振动球磨机对机械化学甲烷化反应的监测结果。
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In-situ monitoring of CO2 methanation: pressure change upon ball-milling of LaNi5 under CO2 and H2
Recently, atmospheric carbon dioxide concentration, which may enhance on-going global warming issue, is increasing rapidly. Here, methanation of atmospheric CO2 has been suggested. However, in the methanation process developed so far, at least 200-300 °C is required with using catalysts like Ni. Therefore, it is desirable to reduce the reaction temperature by different processes from the viewpoint of energy saving and also to avoid deactivation of catalysts at high temperatures. We have recently reported that mechanochemical process of La-Ni based alloys under the presence of CO2 and H2 generates CH4 successfully. But, it has also been suggested by Atom Probe Tomography (APT) analysis carried out in this study, that CO2 might have partially reacted with the LaNi5 powder in the course of ball-milling, yielding different La-oxides, carboxides and hydrocarboxylic species containing La embedded in Ni matrix. These compounds might have acted as effective intermediate phases for the methanation reaction. In order to elucidate the origin of the catalytic activity, in-situ monitoring of the pressure change during the process is necessary; reactivity of CO2 with LaNi5 in the said process should be investigated as well. Herein, monitoring results of mechanochemical methanation reaction by using vibrational ball-mill are presented.
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