Nitrogen-doped mesoporous carbon supported FeCu bimetallic catalyst and its CO hydrogenation performance

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作者
Li, Zhi-Wen [1 ,2 ]
Chen, Cong-Biao [1 ]
Wang, Jun-Gang [1 ]
Lin, Ming-Gui [1 ]
Hou, Bo [1 ]
Jia, Li-Tao [1 ,3 ]
Li, De-Bao [1 ,3 ]
机构
[1] State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan,030001, China
[2] University of Chinese Academy of Sciences, Beijing,100049, China
[3] Dalian National Laboratory for Clean Energy, Dalian,116023, China
关键词
Alkalinity - Carbon - Catalyst selectivity - Catalyst supports - Copper - Doping (additives) - Hydrogenation - Nitrogen;
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摘要
In this work, nitrogen-doped mesoporous carbon (NDMC) was prepared by a hard template method, and the NDMC supported FeCu bimetallic catalysts were prepared by an impregnation method. The physical and chemical properties and CO hydrogenation performance of the catalysts with varying Fe/Cu ratios were studied. The results indicated that Cu-N had strong interaction which directly promoted Cu dispersion on the support. At a relatively high metal loading (45.0%-50.0%), Cu maintained uniform distribution similar to that of N, and the ratios of Fe/Cu on the catalyst surface were smaller than those in the bulk phase, which were different from precipitated Fe-Cu bimetallic catalysts. The XPS results showed that Cu was an electron donor, and the electrons in the Cu-N shifted to Fe. Compared with Fe/NDMC, the reduction of FexCuy/NDMC was facilitated, and their CO hydrogenation activity was significantly increased. Under the pretreatment conditions (H2, 300℃), Fe was not completely reduced, and H might mainly interact with Fe-O in the form of Fe-O-H, while Cu-N interaction was stronger than Cu-H, resulting in a decrease in the ratio of surface active carbon/hydrogen, leading to a gradual increase in C5+ selectivity with the decrease of Fe/Cu ratio. Meanwhile, the introduction of Cu inhibited CO dissociation to some extent, and the electron migration ability of the support to the metal gradually increased with decreasing Fe/Cu ratio, and as a result the surface alkalinity of the catalysts increased with increasing Cu content, leading to further enhancement of C5+ selectivity and alcohol selectivity. © 2019, Science Press. All right reserved.
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页码:709 / 717
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