Tuning of higher alcohol selectivity and productivity in CO hydrogenation reactions over K/MoS2 domains supported on mesoporous activated carbon and mixed MgAl oxide

Micaela Taborga Claure; Song Hai Chai; Sheng Dai; Kinga A. Unocic; Faisal M. Alamgir; Pradeep K. Agrawal; Christopher W. Jones

doi:10.1016/j.jcat.2015.01.015

Tuning of higher alcohol selectivity and productivity in CO hydrogenation reactions over K/MoS₂ domains supported on mesoporous activated carbon and mixed MgAl oxide

Micaela Taborga Claure, Song Hai Chai, Sheng Dai, Kinga A. Unocic, Faisal M. Alamgir, Pradeep K. Agrawal, Christopher W. Jones

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

83 Scopus citations

Abstract

Higher alcohol synthesis from syngas is studied over K/MoS₂ domains supported on mesoporous carbon (C), mixed MgAl oxide (MMO), or mixtures thereof. While the carbon support offers high ethanol productivity, the MMO support yields enhanced C₃₊OH selectivity. MoKMMO-C, whereby Mo is initially contained on MMO then ground with carbon, behaves similar to the parent MoKMMO catalyst, as Mo on MMO has limited mobility during reaction. In contrast, on MoKC-MMO, significant Mo migrates from C to MMO during reaction, giving reactivity associated with Mo species on both supports (high C₃₊OH selectivity and productivity). MoS₂ domain structures are correlated with the selectivity of the catalysts (C₃₊OH selectivity ∼ double MoS₂ layers, total hydrocarbon selectivity ∼ single MoS₂ layers). This study advances the understanding of the support's effect on structure-reactivity relationships for this family of catalysts and introduces a new catalyst composition with desirable reactivity.

Original language	English
Pages (from-to)	88-97
Number of pages	10
Journal	Journal of Catalysis
Volume	324
DOIs	https://doi.org/10.1016/j.jcat.2015.01.015
State	Published - Apr 1 2015

Funding

A portion of this research was conducted at the Center for Nanophase Materials Science, which is sponsored at Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy . Use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract No. DE-AC02-06CH11357 . The authors wish to acknowledge the assistance received at 10-BM-A, B and 12-BM-B. The authors wish to express special thanks to 12-BM-B beamline personnel, Dr. Benjamin Reinhart and Dr. Sungsik Lee. Use of the National Synchrotron Light Source, Brookhaven National Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences , under Contract No. DE-AC02-98CH10886 . The authors also wish to express special thanks to the assistance received from X-18B beamline personnel, Dr. Syed Khalid and Dr. Nebojsa Marinkovic. CWJ, MTC, and SD thank the U.S. DOE Office of Science for partial support of this work (travel, coordination, and partial support for MTC) as part of the Center for Understanding and Control of Acid Gas Evolution of Materials for Energy , an Energy Frontier Research Center, via contract DE-SC0012577 .

Keywords

Activated carbon
Higher alcohols
Mixed metal oxide
Molybdenum sulfide
Potassium
Syngas

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10.1016/j.jcat.2015.01.015

Cite this

@article{af187746ed024db8bc0dcb60c9b67a1d,

title = "Tuning of higher alcohol selectivity and productivity in CO hydrogenation reactions over K/MoS2 domains supported on mesoporous activated carbon and mixed MgAl oxide",

abstract = "Higher alcohol synthesis from syngas is studied over K/MoS2 domains supported on mesoporous carbon (C), mixed MgAl oxide (MMO), or mixtures thereof. While the carbon support offers high ethanol productivity, the MMO support yields enhanced C3+OH selectivity. MoKMMO-C, whereby Mo is initially contained on MMO then ground with carbon, behaves similar to the parent MoKMMO catalyst, as Mo on MMO has limited mobility during reaction. In contrast, on MoKC-MMO, significant Mo migrates from C to MMO during reaction, giving reactivity associated with Mo species on both supports (high C3+OH selectivity and productivity). MoS2 domain structures are correlated with the selectivity of the catalysts (C3+OH selectivity ∼ double MoS2 layers, total hydrocarbon selectivity ∼ single MoS2 layers). This study advances the understanding of the support's effect on structure-reactivity relationships for this family of catalysts and introduces a new catalyst composition with desirable reactivity.",

keywords = "Activated carbon, Higher alcohols, Mixed metal oxide, Molybdenum sulfide, Potassium, Syngas",

author = "{Taborga Claure}, Micaela and Chai, {Song Hai} and Sheng Dai and Unocic, {Kinga A.} and Alamgir, {Faisal M.} and Agrawal, {Pradeep K.} and Jones, {Christopher W.}",

year = "2015",

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doi = "10.1016/j.jcat.2015.01.015",

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journal = "Journal of Catalysis",

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AU - Taborga Claure, Micaela

AU - Chai, Song Hai

AU - Dai, Sheng

AU - Unocic, Kinga A.

AU - Alamgir, Faisal M.

AU - Agrawal, Pradeep K.

AU - Jones, Christopher W.

PY - 2015/4/1

Y1 - 2015/4/1

N2 - Higher alcohol synthesis from syngas is studied over K/MoS2 domains supported on mesoporous carbon (C), mixed MgAl oxide (MMO), or mixtures thereof. While the carbon support offers high ethanol productivity, the MMO support yields enhanced C3+OH selectivity. MoKMMO-C, whereby Mo is initially contained on MMO then ground with carbon, behaves similar to the parent MoKMMO catalyst, as Mo on MMO has limited mobility during reaction. In contrast, on MoKC-MMO, significant Mo migrates from C to MMO during reaction, giving reactivity associated with Mo species on both supports (high C3+OH selectivity and productivity). MoS2 domain structures are correlated with the selectivity of the catalysts (C3+OH selectivity ∼ double MoS2 layers, total hydrocarbon selectivity ∼ single MoS2 layers). This study advances the understanding of the support's effect on structure-reactivity relationships for this family of catalysts and introduces a new catalyst composition with desirable reactivity.

AB - Higher alcohol synthesis from syngas is studied over K/MoS2 domains supported on mesoporous carbon (C), mixed MgAl oxide (MMO), or mixtures thereof. While the carbon support offers high ethanol productivity, the MMO support yields enhanced C3+OH selectivity. MoKMMO-C, whereby Mo is initially contained on MMO then ground with carbon, behaves similar to the parent MoKMMO catalyst, as Mo on MMO has limited mobility during reaction. In contrast, on MoKC-MMO, significant Mo migrates from C to MMO during reaction, giving reactivity associated with Mo species on both supports (high C3+OH selectivity and productivity). MoS2 domain structures are correlated with the selectivity of the catalysts (C3+OH selectivity ∼ double MoS2 layers, total hydrocarbon selectivity ∼ single MoS2 layers). This study advances the understanding of the support's effect on structure-reactivity relationships for this family of catalysts and introduces a new catalyst composition with desirable reactivity.

KW - Activated carbon

KW - Higher alcohols

KW - Mixed metal oxide

KW - Molybdenum sulfide

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