Autothermal reforming of iso-octane and gasoline over Rh-based catalysts: Influence of CeO2/γ-Al2O3-based mixed oxides on hydrogen production

Yeon Gyu Jung; Yongmin Kim; Dae Hyung Lee; Seong Cheol Jang; Suk Woo Nam; Jong Hee Han; Sung An Hong; Dae Ki Choi; Chang Won Yoon

doi:10.1016/j.ijhydene.2013.09.093

Autothermal reforming of iso-octane and gasoline over Rh-based catalysts: Influence of CeO₂/γ-Al₂O₃-based mixed oxides on hydrogen production

Yeon Gyu Jung, Yongmin Kim, Dae Hyung Lee, Seong Cheol Jang, Suk Woo Nam, Jong Hee Han, Sung An Hong, Dae Ki Choi, Chang Won Yoon

Research output: Contribution to journal › Article › peer-review

8 Citations (Scopus)

Abstract

Autothermal reforming (ATR) of iso-octane in the presence of Rh-based catalysts (0.5 wt% of Rh) supported onto γ-Al₂O₃, CeO₂, and ZrO₂ were initially carried out at 700 C with a S/C ratio of 2.0, an O/C ratio of 0.84, and a gas hourly space velocity (GHSV) of 20,000 h^-1. The activity of Rh/γ-Al₂O₃ was found to be higher than Rh/CeO₂ and Rh/ZrO₂, with H₂ and (H₂ + CO) yields of 1.98 and 2.48 mol/mol C, respectively, after 10 h. This Rh/γ-Al₂O₃ material, however, was potentially susceptible to carbon coking and produced 3.5 wt% of carbon deposits following the reforming reaction, as evidenced by C, H, N, and S elemental analysis. In contrast, Rh/CeO₂ catalyst exhibited lower activity but higher stability than Rh/γ-Al₂O₃, with nearly no carbon being formed within 10 h. To combine the superior activity originated from Rh/γ-Al₂O₃ with high stability from Rh/CeO₂, Rh/CeO₂/γ-Al₂O₃ catalysts with different CeO₂ contents were synthesized and examined for the ATR reactions of iso-octane. Compared to Rh/γ-Al₂O ₃, the newly prepared Rh/CeO₂/γ-Al₂O ₃ catalysts (0.5 wt% of Rh and 20 wt% of CeO₂) showed even enhanced activity during 10 h, and H₂ and (H₂ + CO) yields were calculated to be 2.08 and 2.62 mol/mol C, respectively. In addition, as observed with Rh/CeO₂, the catalyst was further found to be stable with less than 0.3 wt% of carbon deposition after 10 h. The Rh/γ-Al₂O₃ and Rh/CeO₂/γ-Al ₂O₃ catalysts were eventually tested for ATR reactions using commercial gasoline that contained sulfur, aromatics, and other impurities. The Rh/γ-Al₂O₃ catalyst was significantly deactivated, showing decreased activity after 4 h, while the Rh/CeO₂/γ-Al₂O₃ catalyst proved to be excellent in terms of stability against coke formation as well as activity towards the desired reforming reaction, maintaining its ability for H ₂ production for 100 h.

Original language	English
Pages (from-to)	15140-15151
Number of pages	12
Journal	International Journal of Hydrogen Energy
Volume	38
Issue number	35
DOIs	https://doi.org/10.1016/j.ijhydene.2013.09.093
Publication status	Published - 2013 Nov 22

Bibliographical note

Funding Information:
This research was supported by the Global Research Laboratory Program through the National Research Foundation of Korea funded by the Ministry of Science, ICT and Future Planning of Republic of Korea . Part of this research was also supported by the National Research Foundation of Korea Grant funded by the Korean Government (MSIP) (2013, University-Institute cooperation program).

Keywords

Autothermal reforming
Gasoline
Hydrogen production
Iso-octane
Mixed oxide supports
Rhodium catalyst

ASJC Scopus subject areas

Renewable Energy, Sustainability and the Environment
Fuel Technology
Condensed Matter Physics
Energy Engineering and Power Technology

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1016/j.ijhydene.2013.09.093

Cite this

Jung, Y. G., Kim, Y., Lee, D. H., Jang, S. C., Nam, S. W., Han, J. H., Hong, S. A., Choi, D. K., & Yoon, C. W. (2013). Autothermal reforming of iso-octane and gasoline over Rh-based catalysts: Influence of CeO₂/γ-Al₂O₃-based mixed oxides on hydrogen production. International Journal of Hydrogen Energy, 38(35), 15140-15151. https://doi.org/10.1016/j.ijhydene.2013.09.093

@article{0713e1a73d9a429d8fd7b52c03ef7d98,

title = "Autothermal reforming of iso-octane and gasoline over Rh-based catalysts: Influence of CeO2/γ-Al2O3-based mixed oxides on hydrogen production",

abstract = "Autothermal reforming (ATR) of iso-octane in the presence of Rh-based catalysts (0.5 wt% of Rh) supported onto γ-Al2O3, CeO2, and ZrO2 were initially carried out at 700 C with a S/C ratio of 2.0, an O/C ratio of 0.84, and a gas hourly space velocity (GHSV) of 20,000 h-1. The activity of Rh/γ-Al2O3 was found to be higher than Rh/CeO2 and Rh/ZrO2, with H2 and (H2 + CO) yields of 1.98 and 2.48 mol/mol C, respectively, after 10 h. This Rh/γ-Al2O3 material, however, was potentially susceptible to carbon coking and produced 3.5 wt% of carbon deposits following the reforming reaction, as evidenced by C, H, N, and S elemental analysis. In contrast, Rh/CeO2 catalyst exhibited lower activity but higher stability than Rh/γ-Al2O3, with nearly no carbon being formed within 10 h. To combine the superior activity originated from Rh/γ-Al2O3 with high stability from Rh/CeO2, Rh/CeO2/γ-Al2O3 catalysts with different CeO2 contents were synthesized and examined for the ATR reactions of iso-octane. Compared to Rh/γ-Al2O 3, the newly prepared Rh/CeO2/γ-Al2O 3 catalysts (0.5 wt% of Rh and 20 wt% of CeO2) showed even enhanced activity during 10 h, and H2 and (H2 + CO) yields were calculated to be 2.08 and 2.62 mol/mol C, respectively. In addition, as observed with Rh/CeO2, the catalyst was further found to be stable with less than 0.3 wt% of carbon deposition after 10 h. The Rh/γ-Al2O3 and Rh/CeO2/γ-Al 2O3 catalysts were eventually tested for ATR reactions using commercial gasoline that contained sulfur, aromatics, and other impurities. The Rh/γ-Al2O3 catalyst was significantly deactivated, showing decreased activity after 4 h, while the Rh/CeO2/γ-Al2O3 catalyst proved to be excellent in terms of stability against coke formation as well as activity towards the desired reforming reaction, maintaining its ability for H 2 production for 100 h.",

keywords = "Autothermal reforming, Gasoline, Hydrogen production, Iso-octane, Mixed oxide supports, Rhodium catalyst",

author = "Jung, {Yeon Gyu} and Yongmin Kim and Lee, {Dae Hyung} and Jang, {Seong Cheol} and Nam, {Suk Woo} and Han, {Jong Hee} and Hong, {Sung An} and Choi, {Dae Ki} and Yoon, {Chang Won}",

note = "Funding Information: This research was supported by the Global Research Laboratory Program through the National Research Foundation of Korea funded by the Ministry of Science, ICT and Future Planning of Republic of Korea . Part of this research was also supported by the National Research Foundation of Korea Grant funded by the Korean Government (MSIP) (2013, University-Institute cooperation program).",

year = "2013",

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doi = "10.1016/j.ijhydene.2013.09.093",

language = "English",

volume = "38",

pages = "15140--15151",

journal = "International Journal of Hydrogen Energy",

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TY - JOUR

T1 - Autothermal reforming of iso-octane and gasoline over Rh-based catalysts

T2 - Influence of CeO2/γ-Al2O3-based mixed oxides on hydrogen production

AU - Jung, Yeon Gyu

AU - Kim, Yongmin

AU - Lee, Dae Hyung

AU - Jang, Seong Cheol

AU - Nam, Suk Woo

AU - Han, Jong Hee

AU - Hong, Sung An

AU - Choi, Dae Ki

AU - Yoon, Chang Won

N1 - Funding Information: This research was supported by the Global Research Laboratory Program through the National Research Foundation of Korea funded by the Ministry of Science, ICT and Future Planning of Republic of Korea . Part of this research was also supported by the National Research Foundation of Korea Grant funded by the Korean Government (MSIP) (2013, University-Institute cooperation program).

PY - 2013/11/22

Y1 - 2013/11/22

N2 - Autothermal reforming (ATR) of iso-octane in the presence of Rh-based catalysts (0.5 wt% of Rh) supported onto γ-Al2O3, CeO2, and ZrO2 were initially carried out at 700 C with a S/C ratio of 2.0, an O/C ratio of 0.84, and a gas hourly space velocity (GHSV) of 20,000 h-1. The activity of Rh/γ-Al2O3 was found to be higher than Rh/CeO2 and Rh/ZrO2, with H2 and (H2 + CO) yields of 1.98 and 2.48 mol/mol C, respectively, after 10 h. This Rh/γ-Al2O3 material, however, was potentially susceptible to carbon coking and produced 3.5 wt% of carbon deposits following the reforming reaction, as evidenced by C, H, N, and S elemental analysis. In contrast, Rh/CeO2 catalyst exhibited lower activity but higher stability than Rh/γ-Al2O3, with nearly no carbon being formed within 10 h. To combine the superior activity originated from Rh/γ-Al2O3 with high stability from Rh/CeO2, Rh/CeO2/γ-Al2O3 catalysts with different CeO2 contents were synthesized and examined for the ATR reactions of iso-octane. Compared to Rh/γ-Al2O 3, the newly prepared Rh/CeO2/γ-Al2O 3 catalysts (0.5 wt% of Rh and 20 wt% of CeO2) showed even enhanced activity during 10 h, and H2 and (H2 + CO) yields were calculated to be 2.08 and 2.62 mol/mol C, respectively. In addition, as observed with Rh/CeO2, the catalyst was further found to be stable with less than 0.3 wt% of carbon deposition after 10 h. The Rh/γ-Al2O3 and Rh/CeO2/γ-Al 2O3 catalysts were eventually tested for ATR reactions using commercial gasoline that contained sulfur, aromatics, and other impurities. The Rh/γ-Al2O3 catalyst was significantly deactivated, showing decreased activity after 4 h, while the Rh/CeO2/γ-Al2O3 catalyst proved to be excellent in terms of stability against coke formation as well as activity towards the desired reforming reaction, maintaining its ability for H 2 production for 100 h.

AB - Autothermal reforming (ATR) of iso-octane in the presence of Rh-based catalysts (0.5 wt% of Rh) supported onto γ-Al2O3, CeO2, and ZrO2 were initially carried out at 700 C with a S/C ratio of 2.0, an O/C ratio of 0.84, and a gas hourly space velocity (GHSV) of 20,000 h-1. The activity of Rh/γ-Al2O3 was found to be higher than Rh/CeO2 and Rh/ZrO2, with H2 and (H2 + CO) yields of 1.98 and 2.48 mol/mol C, respectively, after 10 h. This Rh/γ-Al2O3 material, however, was potentially susceptible to carbon coking and produced 3.5 wt% of carbon deposits following the reforming reaction, as evidenced by C, H, N, and S elemental analysis. In contrast, Rh/CeO2 catalyst exhibited lower activity but higher stability than Rh/γ-Al2O3, with nearly no carbon being formed within 10 h. To combine the superior activity originated from Rh/γ-Al2O3 with high stability from Rh/CeO2, Rh/CeO2/γ-Al2O3 catalysts with different CeO2 contents were synthesized and examined for the ATR reactions of iso-octane. Compared to Rh/γ-Al2O 3, the newly prepared Rh/CeO2/γ-Al2O 3 catalysts (0.5 wt% of Rh and 20 wt% of CeO2) showed even enhanced activity during 10 h, and H2 and (H2 + CO) yields were calculated to be 2.08 and 2.62 mol/mol C, respectively. In addition, as observed with Rh/CeO2, the catalyst was further found to be stable with less than 0.3 wt% of carbon deposition after 10 h. The Rh/γ-Al2O3 and Rh/CeO2/γ-Al 2O3 catalysts were eventually tested for ATR reactions using commercial gasoline that contained sulfur, aromatics, and other impurities. The Rh/γ-Al2O3 catalyst was significantly deactivated, showing decreased activity after 4 h, while the Rh/CeO2/γ-Al2O3 catalyst proved to be excellent in terms of stability against coke formation as well as activity towards the desired reforming reaction, maintaining its ability for H 2 production for 100 h.

KW - Autothermal reforming

KW - Gasoline

KW - Hydrogen production

KW - Iso-octane

KW - Mixed oxide supports

KW - Rhodium catalyst

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