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通过锰调谐稳定的ε-FeC催化剂,以抑制高温烯烃合成中C1副产物的选择性。

Stabilized ε-FeC catalyst with Mn tuning to suppress C1 byproduct selectivity for high-temperature olefin synthesis.

作者信息

Qian Fei, Bai Jiawei, Cai Yi, Yang Hui, Cao Xue-Min, Liu Xingchen, Liu Xing-Wu, Yang Yong, Li Yong-Wang, Ma Ding, Wen Xiao-Dong

机构信息

State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, 030001, China.

National Energy Center for Coal to Liquids, Synfuels China Co., Ltd., Huairou District, Beijing, 101400, China.

出版信息

Nat Commun. 2024 Jun 15;15(1):5128. doi: 10.1038/s41467-024-49472-x.

Abstract

Accurately controlling the product selectivity in syngas conversion, especially increasing the olefin selectivity while minimizing C1 byproducts, remains a significant challenge. Epsilon FeC is deemed a promising candidate catalyst due to its inherently low CO selectivity, but its use is hindered by its poor high-temperature stability. Herein, we report the successful synthesis of highly stable ε-FeC through a N-induced strategy utilizing pyrolysis of Prussian blue analogs (PBAs). This catalyst, with precisely controlled Mn promoter, not only achieved an olefin selectivity of up to 70.2% but also minimized the selectivity of C1 byproducts to 19.0%, including 11.9% CO and 7.1% CH. The superior performance of our ε-FeC-xMn catalysts, particularly in minimizing CO formation, is largely attributed to the interface of dispersed MnO cluster and ε-FeC, which crucially limits CO to CO conversion. Here, we enhance the carbon efficiency and economic viability of the olefin production process while maintaining high catalytic activity.

摘要

精确控制合成气转化中的产物选择性,尤其是提高烯烃选择性同时将C1副产物降至最低,仍然是一项重大挑战。ε-FeC因其固有的低CO选择性而被认为是一种有前景的候选催化剂,但其高温稳定性较差限制了其应用。在此,我们报道了通过利用普鲁士蓝类似物(PBAs)热解的N诱导策略成功合成了高度稳定的ε-FeC。这种具有精确控制的Mn促进剂的催化剂,不仅实现了高达70.2%的烯烃选择性,还将C1副产物的选择性降至19.0%,其中包括11.9%的CO和7.1%的CH。我们的ε-FeC-xMn催化剂的优异性能,特别是在将CO生成降至最低方面,很大程度上归因于分散的MnO团簇与ε-FeC的界面,这至关重要地限制了CO向CO的转化。在此,我们在保持高催化活性的同时提高了烯烃生产过程的碳效率和经济可行性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/feae/11180106/01acc4263f89/41467_2024_49472_Fig1_HTML.jpg

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