Carbon Dioxide Hydrogenation under Subcritical and Supercritical Conditions in the Presence of 15% Fe/SiO 2 Catalyst

被引：13

作者：

Evdokimenko N.D. ^{[1
]}

Kim K.O. ^{[2
]}

Kapustin G.I. ^{[1
]}

Davshan N.A. ^{[1
]}

Kustov A.L. ^{[1
,2
]}

机构：

[1] Zelinsky Institute of Organic Chemistry, Russian Academy of Sciences, Moscow

[2] Moscow State University, Moscow

来源：

Catalysis in Industry | 2018年 / 10卷 / 04期

关键词：

carbon dioxide; catalysis; hydrogenation; iron catalyst; supercritical conditions; supercritical fluid;

D O I：

10.1134/S2070050418040062

中图分类号：

学科分类号：

摘要：

Abstract: Results are presented from a comparative study of CO 2 hydrogenation under gas-phase and supercritical conditions for CO 2 in the presence of 15% Fe/SiO 2 catalyst. The reaction is studied in the temperature range of 300–500°C at atmospheric pressure under gas-phase conditions and at a pressure of 95 atm under supercritical conditions at an Н 2 : СО 2 molar ratio of 2 : 1. It is found that the process proceeding under supercritical conditions lowers CO selectivity from 90–95 to 30–50% over the range of temperatures and raises (up to 60%) the hydrocarbon selectivity. In contrast to gas-phase hydrogenation, the formation of alcohols is observed in the reaction under supercritical conditions. Using a combination of thermogravimetry, differential thermogravimetry, and differential thermal analysis (TG–DTG–DTA), it is shown that the process proceeding under supercritical conditions results in a 2.2-fold drop in the amount of carbon-like deposits on the catalyst surface. X-ray diffraction analysis shows that under gas-phase process conditions, graphite-like structures form on the catalyst surface; this effect is not observed under supercritical conditions. The developed catalyst and the process for CO 2 hydrogenation can be recommended for the further modification and improvement of the properties of a catalyst based on iron nanoparticles that is much (10–100 times) cheaper than the previously reported CO 2 hydrogenation catalysts. © 2018, Pleiades Publishing, Ltd.

引用

页码：288 / 293

页数：5

共 30 条

[1]

Leitner W., Acc. Chem. Res., 35, pp. 746-756, (2002)

[2]

Kruse A., Vogel H., Chem. Eng. Technol., 31, pp. 23-32, (2008)

[3]

Utsis N., Vidruk-Nehemya R., Landau M.V., Herskowitz M., Faraday Discuss., 188, pp. 545-563, (2016)

[4]

da Ponte M.N., J. Supercrit. Fluids, 47, 3, pp. 344-350, (2009)

[5]

Liu R., Zhang P., Zhang S., Yan T., Xin J., Zhang X., Rev. Chem. Eng., 32, pp. 587-609, (2016)

[6]

Rakitin M.Y., Doluda V.Y., Tereshchenkov A.Y., Demidenko G.N., Lakina N.V., Matveeva V.G., Sul'man M.G., Sul'man E.M., Catal. Ind., 7, pp. 1-5, (2015)

[7]

Ramsey E., Sun Q., Zhang Z., Zhang C., Gou W., J. Environ. Sci., 21, pp. 720-726, (2009)

[8]

Wang W., Wang S., Ma X., Gong J., Chem. Soc. Rev., 40, pp. 3703-3727, (2011)

[9]

Gao P., Li S., Bu X., Dang S., Liu Z., Wang H., Zhong L., Qiu M., Yang C., Cai J., Wei W., Sun Y., Nat. Chem., 9, pp. 1019-1024, (2017)

[10]

Wang X., Shi H., Szangi J., Nat. Commun., 8, pp. 513-519, (2017)

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