Graphitic mesoporous carbon as a support of promoted Rh catalysts for hydrogenation of carbon monoxide to ethanol

Song Hai Chai; Jane Y. Howe; Xiqing Wang; Michelle Kidder; Viviane Schwartz; Melissa L. Golden; Steven H. Overbury; Sheng Dai; De En Jiang

doi:10.1016/j.carbon.2011.11.036

Graphitic mesoporous carbon as a support of promoted Rh catalysts for hydrogenation of carbon monoxide to ethanol

Song Hai Chai, Jane Y. Howe, Xiqing Wang, Michelle Kidder, Viviane Schwartz, Melissa L. Golden, Steven H. Overbury, Sheng Dai, De En Jiang

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

42 Scopus citations

Abstract

Graphitic mesoporous carbon (GMC), prepared through high-temperature graphitization of soft-templated amorphous mesoporous carbon (AMC), was used as the support for Mn, Li, and Fe triple-promoted Rh catalysts for CO hydrogenation to ethanol. The use of GMC results in C ₂H ₅OH selectivity and formation rate comparable to nonporous SiO ₂ support along with a significant inhibition on the formation of undesired CH ₄ and light hydrocarbons at the expense of appreciable amounts of CO ₂ produced. The better catalytic performance of promoted-Rh/GMC than those supported on other carbon allotropes (AMC and non-porous graphitic carbon black) seems to be associated with the specific graphitic structure and mesoporosity of GMC. The surface modification of GMC by wet oxidation leads to considerable increases in C ₂H ₅OH selectivity and formation rate. The modified GMC as a support shows substantially greater CO ₂-free selectivity for C ₂H ₅OH than the SiO ₂.

Original language	English
Pages (from-to)	1574-1582
Number of pages	9
Journal	Carbon
Volume	50
Issue number	4
DOIs	https://doi.org/10.1016/j.carbon.2011.11.036
State	Published - Apr 2012

Funding

This research was sponsored by the laboratory-directed research and development (LDRD) program of Oak Ridge National Laboratory, managed and operated by UT-Battelle, LLC. A portion of this research was conducted at the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Division of Scientific User Facilities, U.S. Department of Energy. Dr. Zili Wu and Dr. Gabriel M. Veith were acknowledged for catalyst characterizations.

Funders	Funder number
U.S. Department of Energy
Basic Energy Sciences
Oak Ridge National Laboratory

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10.1016/j.carbon.2011.11.036

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title = "Graphitic mesoporous carbon as a support of promoted Rh catalysts for hydrogenation of carbon monoxide to ethanol",

abstract = "Graphitic mesoporous carbon (GMC), prepared through high-temperature graphitization of soft-templated amorphous mesoporous carbon (AMC), was used as the support for Mn, Li, and Fe triple-promoted Rh catalysts for CO hydrogenation to ethanol. The use of GMC results in C 2H 5OH selectivity and formation rate comparable to nonporous SiO 2 support along with a significant inhibition on the formation of undesired CH 4 and light hydrocarbons at the expense of appreciable amounts of CO 2 produced. The better catalytic performance of promoted-Rh/GMC than those supported on other carbon allotropes (AMC and non-porous graphitic carbon black) seems to be associated with the specific graphitic structure and mesoporosity of GMC. The surface modification of GMC by wet oxidation leads to considerable increases in C 2H 5OH selectivity and formation rate. The modified GMC as a support shows substantially greater CO 2-free selectivity for C 2H 5OH than the SiO 2.",

author = "Chai, {Song Hai} and Howe, {Jane Y.} and Xiqing Wang and Michelle Kidder and Viviane Schwartz and Golden, {Melissa L.} and Overbury, {Steven H.} and Sheng Dai and Jiang, {De En}",

year = "2012",

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journal = "Carbon",

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T1 - Graphitic mesoporous carbon as a support of promoted Rh catalysts for hydrogenation of carbon monoxide to ethanol

AU - Chai, Song Hai

AU - Howe, Jane Y.

AU - Wang, Xiqing

AU - Kidder, Michelle

AU - Schwartz, Viviane

AU - Golden, Melissa L.

AU - Overbury, Steven H.

AU - Dai, Sheng

AU - Jiang, De En

PY - 2012/4

Y1 - 2012/4

N2 - Graphitic mesoporous carbon (GMC), prepared through high-temperature graphitization of soft-templated amorphous mesoporous carbon (AMC), was used as the support for Mn, Li, and Fe triple-promoted Rh catalysts for CO hydrogenation to ethanol. The use of GMC results in C 2H 5OH selectivity and formation rate comparable to nonporous SiO 2 support along with a significant inhibition on the formation of undesired CH 4 and light hydrocarbons at the expense of appreciable amounts of CO 2 produced. The better catalytic performance of promoted-Rh/GMC than those supported on other carbon allotropes (AMC and non-porous graphitic carbon black) seems to be associated with the specific graphitic structure and mesoporosity of GMC. The surface modification of GMC by wet oxidation leads to considerable increases in C 2H 5OH selectivity and formation rate. The modified GMC as a support shows substantially greater CO 2-free selectivity for C 2H 5OH than the SiO 2.

AB - Graphitic mesoporous carbon (GMC), prepared through high-temperature graphitization of soft-templated amorphous mesoporous carbon (AMC), was used as the support for Mn, Li, and Fe triple-promoted Rh catalysts for CO hydrogenation to ethanol. The use of GMC results in C 2H 5OH selectivity and formation rate comparable to nonporous SiO 2 support along with a significant inhibition on the formation of undesired CH 4 and light hydrocarbons at the expense of appreciable amounts of CO 2 produced. The better catalytic performance of promoted-Rh/GMC than those supported on other carbon allotropes (AMC and non-porous graphitic carbon black) seems to be associated with the specific graphitic structure and mesoporosity of GMC. The surface modification of GMC by wet oxidation leads to considerable increases in C 2H 5OH selectivity and formation rate. The modified GMC as a support shows substantially greater CO 2-free selectivity for C 2H 5OH than the SiO 2.

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DO - 10.1016/j.carbon.2011.11.036

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SP - 1574

EP - 1582

JO - Carbon

JF - Carbon

IS - 4

ER -

Graphitic mesoporous carbon as a support of promoted Rh catalysts for hydrogenation of carbon monoxide to ethanol

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