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Regulating iron species compositions by Fe-Al interaction in CO2 hydrogenation
Journal of Catalysis ( IF 7.3 ) Pub Date : 2022-06-24 , DOI: 10.1016/j.jcat.2022.06.030
Minjie Xu , Xianglin Liu , Guiyao Song , Yingying Cai , Bianfang Shi , Yitao Liu , Xiaoxu Ding , Zixu Yang , Pengfei Tian , Chenxi Cao , Jing Xu

Different iron species exhibit distinct activity and selectivity in CO2 hydrogenation reaction. Herein, by controlling calcination temperature, Fe-Al interaction in Na promoted Fe-Al catalysts has been regulated, which further leads to various compositions of iron oxide (FeOx) and iron carbides (Fe7C3 and Fe5C2) after CO activation and CO2 hydrogenation reaction. The phase compositions and structures of Fe-Al catalysts are carefully distinguished by multiple characterizations, including XRD, XPS, MES and TEM, and the reactivity of different phases is studied with the combination of experiments (kinetics, TP and in situ DRIFTS) and Density Functional Theory (DFT) calculations. Our FeAl350 with the highest FeCx content shows the highest CO2 conversion of 48.2% and the lowest CO selectivity of 10.1%, and FeAl900 with the highest Fe5C2 / FeCx ratio presents the highest C5+ selectivity of 44.6%. Finally, a correlation between different compositions of iron species with the activity and selectivity of Fe-based for CO2 hydrogenation to olefins was established.



中文翻译:

在 CO2 加氢中通过 Fe-Al 相互作用调节铁物种组成

不同的铁物种在CO 2加氢反应中表现出不同的活性和选择性。在此,通过控制煅烧温度,可以调节 Na 促进的 Fe-Al 催化剂中的 Fe-Al 相互作用,进而导致氧化铁 (FeO x ) 和碳化铁 (Fe 7 C 3和 Fe 5 C 2 )的不同组成。 CO活化和CO 2加氢反应。通过 XRD、XPS、MES 和 TEM 等多种表征仔细区分 Fe-Al 催化剂的相组成和结构,并结合实验(动力学、TP 和原位)研究不同相的反应性漂移)和密度泛函理论(DFT)计算。我们的 FeC x含量最高的 FeAl350 的 CO 2转化率最高,为 48.2%,CO 选择性最低,为 10.1%,而 Fe 5 C 2 / FeC x比率最高的 FeAl900 的 C 5+选择性最高,为 44.6%。最后,建立了不同铁组分组成与铁基CO 2加氢制烯烃的活性和选择性之间的相关性。

更新日期:2022-06-24
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