Engineering of Ruthenium-Iron Oxide Colloidal Heterostructures: Improved Yields in CO2 Hydrogenation to Hydrocarbons
Engineering of Ruthenium-Iron Oxide Colloidal Heterostructures: Improved Yields in CO2 Hydrogenation to Hydrocarbons
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DOI：
10.1002/anie.201910579
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发表时间：
2019-10-17
影响因子：
16.6
通讯作者：
Cargnello, Matteo
中科院分区：
文献类型：
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作者：
Aitbekova, Aisulu;Goodman, Emmett D.;Cargnello, Matteo
催化二氧化碳还原为燃料和化学品是减少温室气体排放的主要目标。一种方法利用逆水煤气变换反应，然后进行费托合成，而铁是该过程的众所周知的候选者。已经进行了一些尝试来修改和提高其反应性，但取得的成功有限。现在，使用钌铁氧化物胶体异二聚体，两相之间的紧密接触通过近端氢溢出效应促进氧化铁的还原，从而形成钌铁核壳结构，该结构在比裸铁催化剂低得多的温度下对反应具有活性。此外，通过设计氧化铁壳厚度，与异二聚体相比，烃产量增加了四倍。这项工作展示了胶体异质结构的合理设计如何能够显着提高材料在二氧化碳转化过程中的催化性能。
Catalytic CO2 reduction to fuels and chemicals is a major pursuit in reducing greenhouse gas emissions. One approach utilizes the reverse water-gas shift reaction, followed by Fischer-Tropsch synthesis, and iron is a well-known candidate for this process. Some attempts have been made to modify and improve its reactivity, but resulted in limited success. Now, using ruthenium-iron oxide colloidal heterodimers, close contact between the two phases promotes the reduction of iron oxide via a proximal hydrogen spillover effect, leading to the formation of ruthenium-iron core-shell structures active for the reaction at significantly lower temperatures than in bare iron catalysts. Furthermore, by engineering the iron oxide shell thickness, a fourfold increase in hydrocarbon yield is achieved compared to the heterodimers. This work shows how rational design of colloidal heterostructures can result in materials with significantly improved catalytic performance in CO2 conversion processes.