当前位置: X-MOL 学术J. CO2 Util. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Are Fe based catalysts an upcoming alternative to Ni in CO2 methanation at elevated pressure?
Journal of CO2 Utilization ( IF 7.2 ) Pub Date : 2020-04-24 , DOI: 10.1016/j.jcou.2020.101175
Tanja Franken , Andre Heel

The raise of regenerative but unsteadily produced energy demands a highly flexible way to store the energy for time periods when less energy is produced than consumed. In the current study, it is investigated if catalysts based on environmentally more attractive and less hazardous to health Fe might be able to be considered as an alternative to Ni catalysts in the CO2 methanation at elevated pressure. For this a set of catalysts with 1–10 wt % Fe supported on the zeolite 13X is analysed in CO2 methanation at 1–15 bar. The trends of activity as well as selectivity with varying Fe loading and pressure are presented. Correlation with thorough characterization of the materials shows that a very high dispersion of Fe in octahedral sites within the zeolite is necessary to generate CH4 as the main reaction product and suppress the Fischer–Tropsch activity towards CC coupling reactions at elevated pressure. Especially with low Fe loading such as 1 wt % high reaction rates of 42 mmol(CO2)/(mol(Fe)∙s) with a CH4 selectivity of 76 % at 300 °C and 10 bar are obtained. In contrast to that, highly Fe loaded catalysts tend to form increasing amounts of Fischer–Tropsch products at increasing pressure. In addition, highly Fe-loaded catalysts are much more susceptible to destruction of the zeolite under reaction conditions. At the same time, highly loaded catalysts form a Fe3C shell around the remaining support. Hence, avoiding the formation of a Fe3C phase is crucial for high CH4 selectivity. The results presented here therefore show that catalysts with a very high Fe-dispersion in particular can gain considerably in importance as alternatives to Ni-methanation catalysts at elevated pressure.



中文翻译:

铁基催化剂是否会在高压下成为CO 2甲烷化中Ni的替代品?

可再生但不稳定产生的能量的增加需要一种高度灵活的方式来存储能量,该时间用于产生的能量少于消耗的能量。在当前的研究中,研究了在高压下将CO 2甲烷化中基于环境的吸引力更大,对健康危害较小的催化剂是否可以被视为Ni催化剂的替代品。为此,在1-15 bar的CO 2甲烷化条件下分析了负载在13X沸石上的1-10 wt%Fe的一组催化剂。介绍了随着铁负载和压力的变化,活性以及选择性的变化趋势。与材料的全面表征相关,表明Fe在沸石的八面体位点中非常高的分散性对于生成CH是必要的4作为主要反应产物,并抑制了费-托在高压下对C C偶联反应的活性。尤其是在Fe含量低(例如1 wt%)的情况下,在300°C和10 bar的压力下,CH 4选择性达到76%时,反应速率高达42 mmol(CO 2)/(mol(Fe)∙s)。与此相反,高铁负载的催化剂往往会在越来越高的压力下形成越来越多的费托产品。另外,高铁负载的催化剂在反应条件下更易于破坏沸石。同时,高负载的催化剂在剩余的载体周围形成Fe 3 C壳。因此,对于高CH 4而言,避免形成Fe 3 C相至关重要选择性。因此,在此给出的结果表明,具有非常高的铁分散性的催化剂作为高压下的镍甲烷化催化剂的替代品,尤其具有重要的意义。

更新日期:2020-04-24
down
wechat
bug