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Effect of EDTA-2Na modification on Fe-Co/Al2O3 for hydrogenation of carbon dioxide to lower olefins and gasoline

Journal 2020 · IF 5.993 · 发表于 2020 年 11 月 10 日
作者: Chengyi Dai,Xiao Zhao,Borui Hu,Xinbao Zhang,Qunxing Luo,Xinwen Guo,Xiaoxun Ma
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摘要

Capturing and utilization of carbon dioxide (CO 2 ) not only leads to effective use of carbon resources, but also alleviates environmental pollution caused by increasing concentration of CO 2 , thus making it a hot research topic in recent years. In this study, a series of highly dispersed iron-cobalt (Fe-Co) catalysts was prepared by ethylenediaminetetraacetic acid disodium salt (EDTA-2Na) modification, which could efficiently convert CO 2 into high value-added chemicals (C 2 -C 4 = and C 5 -C 11 ). X-ray diffraction (XRD) analysis showed that the addition of a small amount of Co and EDTA-2Na contributed to enhance the sintering resistance of Fe species. During the calcination process, EDTA 4− can be decomposed into small organic molecules with reducibility, thus promoting the reduction of iron species. The CO temperature-programmed desorption (CO-TPD) results showed that cobalt enhanced the adsorption and activation of intermediate CO on Na x Fe-Co catalyst, thereby promoting the catalytic conversion of CO 2 . The complexation of EDTA promotes the synergistic effect of Fe-Co bimetals, enhances the chemical adsorption of CO 2 . Sodium in EDTA-2Na promotes the surface basicity of the catalysts, which is favored for improving the product distribution of hydrocarbons. At lower H 2 /CO 2 (1/1) ratio, the EDTA-2Na modified Fe-Co/Al 2 O 3 catalyst exhibited high conversion of CO 2 (32.8 %) and excellent selectivity toward high value-added chemicals. The selectivity of by-product CO was only 8.1 %; and C 2 -C 4 = (32.5 %) and C 5 -C 11 (46.3 %) accounted for ∼79 % selectivity among the hydrocarbons generated.