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Highly Selective Olefin Production from CO2 Hydrogenation on Iron Catalysts: A Subtle Synergy between Manganese and Sodium Additives.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-08-18 , DOI: 10.1002/anie.202009620
Yao Xu 1 , Peng Zhai 1 , Yuchen Deng 1 , Jinglin Xie 1 , Xi Liu 2, 3 , Shuai Wang 4 , Ding Ma 1
Affiliation  

Mn and Na additives have been widely studied to improve the efficiency of CO2 hydrogenation to valuable olefins on Fe catalysts, but their effects on the catalytic properties and mechanism are still under vigorous debate. This study shows that Fe‐based catalysts with moderate Mn and Na contents are highly selective for CO2 hydrogenation to olefins, together with low selectivities for both CO and CH4 and much improved space‐time olefin yields compared to state‐of‐the‐art catalysts. Combined kinetic assessment and quasi in situ characterizations further unveil that the sole presence of Mn suppresses the activity of Fe catalysts because of the close contact between Fe and Mn, whereas the introduction of Na mediates the Fe–Mn interaction and provides strong basic sites. This subtle synergy between Na and Mn sheds light on the importance of the interplay of multiple additives that could bring an enabling strategy to improve catalytic activity and selectivity.

中文翻译:

铁催化剂在CO2加氢中高选择性生产烯烃:锰和钠添加剂之间的微妙协同作用。

Mn和Na添加剂已被广泛研究以提高在Fe催化剂上将CO 2加氢成有价值的烯烃的效率,但它们对催化性能和机理的影响仍在激烈争论中。这项研究表明,Mn和Na含量适中的铁基催化剂对于CO 2加氢成烯烃的选择性高,同时对CO和CH 4的选择性低。与最先进的催化剂相比,时空烯烃产率大大提高。结合动力学评估和准原位表征进一步揭示,由于Fe和Mn之间的紧密接触,Mn的唯一存在抑制了Fe催化剂的活性,而Na的引入介导了Fe-Mn相互作用并提供了牢固的碱性位点。Na和Mn之间这种微妙的协同作用揭示了多种添加剂相互作用的重要性,这可以带来改善催化活性和选择性的可行策略。
更新日期:2020-08-18
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