Enhanced stability of Fe-modified CuO-ZnO-ZrO2-Al2O3/HZSM-5 bifunctional catalysts for dimethyl ether synthesis from CO2 hydrogenation

Fan, Xiao; Ren, Shoujie; Jin, Baitang; Li, Shiguang; Yu, Miao; Liang, Xinhua

doi:10.1016/j.cjche.2020.11.031

Enhanced stability of Fe-modified CuO-ZnO-ZrO₂-Al₂O₃/HZSM-5 bifunctional catalysts for dimethyl ether synthesis from CO₂ hydrogenation

Journal Article · Wed Dec 30 23:00:00 EST 2020 · Chinese Journal of Chemical Engineering

DOI:https://doi.org/10.1016/j.cjche.2020.11.031· OSTI ID:1976963

^[1]; Ren, Shoujie ^[2]; Jin, Baitang ^[2]; Li, Shiguang ^[3]; Yu, Miao ^[4]; ^[2]

Missouri University of Science and Technology, Rolla, MO (United States); OSTI
Missouri University of Science and Technology, Rolla, MO (United States)
Gas Technology Institute, Des Plaines, IL (United States)
Rensselaer Polytechnic Institute, Troy, NY (United States)

In this report a series of iron (Fe) modified CuO-ZnO-ZrO₂-Al₂O₃ (CZZA) catalysts, with various Fe loadings, were prepared using a co-precipitation method. A bifunctional catalyst, consisting of Fe-modified CZZA and HZSM-5, was studied for dimethyl ether (DME) synthesis via CO₂ hydrogenation. The effects of Fe loading, reaction temperature, reaction pressure, space velocity, and concentrations of precursor for the synthesis of the Fe-modified CZZA catalyst on the catalytic activity of DME synthesis were investigated. Long-term stability tests showed that Fe modification of the CZZA catalyst improved the catalyst stability for DME synthesis via CO₂ hydrogenation. The activity loss, in terms of DME yield, was significantly reduced from 4.2% to 1.4% in a 100 h run of reaction, when the Fe loading amount was 0.5 (molar ratio of Fe to Cu). An analysis of hydrogen temperature programmed reduction revealed that the introduction of Fe improved the reducibility of the catalysts, due to assisted adsorption of H₂ on iron oxide. The good stability of Fe-modified CZZA catalysts in the DME formation was most likely attributed to oxygen spillover that was introduced by the addition of iron oxide. This could have inhibited the oxidation of the Cu surface and enhanced the thermal stability of copper during long-term reactions.

View Accepted Manuscript (DOE)

Research Organization:: Gas Technology Institute, Des Plaines, IL (United States); Missouri University of Science and Technology, Rolla, MO (United States)

Sponsoring Organization:: USDOE Advanced Research Projects Agency - Energy (ARPA-E)

Grant/Contract Number:: AR0000806

OSTI ID:: 1976963

Alternate ID(s):: OSTI ID: 1830269

Journal Information:: Chinese Journal of Chemical Engineering, Journal Name: Chinese Journal of Chemical Engineering Journal Issue: C Vol. 38; ISSN 1004-9541

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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