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Hoflund, Gar B.; Epling, William S.; Minahan, David M.

doi:10.1023/a:1018922802698

Cited by 36 publications

(16 citation statements)

References 9 publications

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“…For example, the Cu/ZnO catalyst, which is a renowned catalyst for methanol synthesis from syngas [1], gives a higher yield of higher alcohols such as propanol and butanol when the catalyst is doped with the Cs atoms [2,3]. A similar effect is also found for the K-promoted ZnO catalyst, which is found to be efficient for isobutanol synthesis, in sharp contrast to the undoped ZnO catalyst, which does not yield isobutanol [4,5]. A precise role of doped AM's in these catalytic reactions has not been fully understood.…”

Section: Introductionmentioning

confidence: 78%

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Alkali-Metals on ZnO(10-10) Studied by Low-Energy Electron Diffraction and Photoelectron Spectroscopy

Ozawa

Satō

Oba

et al. 2005

e-J. Surf. Sci. Nanotechnol.

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The geometric and electronic properties of alkali metals (Na and Cs) on ZnO(1010) are investigated by means of photoelectron spectroscopy and low energy electron diffraction (LEED). Growth of the Na overlayer on ZnO(1010) at room temperature is characterized by layer-by-layer growth or monolayer growth followed by three-dimensional cluster growth. The Na adatoms in the first layer are in a cationic state, and the metallic phase is formed on top of the first cationic layer. Although Na deposition at room temperature does not yield any long-range ordered superstructure, annealing the Na-covered surface results in a (1×3) LEED pattern, and we propose the formation of the Na atomic chains along the Zn-O dimer rows. For the Cs adsorption system, the disordered overlayer by ionized Cs adatoms is also formed throughout the submonolayer coverage region. Unlike the Na adsorption system, heat treatment of the Cs-covered surface does not yield any ordered structure until all Cs adatoms desorb from the surface.

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Section: Introductionmentioning

confidence: 78%

“…A precise role of doped AM's in these catalytic reactions has not been fully understood. Thus, it is important to study the adsorption state of AM's and their behavior on the ZnO surface, especially at working temperatures between 500 and 700 K [1][2][3][4][5].…”

Section: Introductionmentioning

confidence: 99%

Alkali-Metals on ZnO(10-10) Studied by Low-Energy Electron Diffraction and Photoelectron Spectroscopy

Ozawa

Satō

Oba

et al. 2005

e-J. Surf. Sci. Nanotechnol.

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“…Higher alcohol synthesis has been investigated with different families of heterogeneous catalysts including noble metal Rh-based catalysts [3][4][5][6][7][8][9][10][11], modified Cu-based methanol synthesis catalysts [12][13][14][15][16], and modified FT catalysts based on Co, Ru, and Fe [5,8,[17][18][19]. A particularly promising non-noble metal family of catalysts, MoS 2 -based catalysts modified with potassium [20,21], has been widely studied due to its resistance to sulfur poisoning, less severe coke deposition, and ability to form higher alcohols with a high selectivity to ethanol.…”

Section: Introductionmentioning

confidence: 99%

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

Claure

Chai

Dai

et al. 2015

Journal of Catalysis

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a b s t r a c tHigher alcohol synthesis from syngas is studied over K/MoS 2 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 C 3+ 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 C 3+ OH selectivity and productivity). MoS 2 domain structures are correlated with the selectivity of the catalysts (C 3+ OH selectivity $ double MoS 2 layers, total hydrocarbon selectivity $ single MoS 2 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.

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“…This synthesis route has been investigated with different families of catalysts including noble metal Rh-based catalysts [1][2][3][4][5][6], alkali modified methanol synthesis catalysts over Cu based catalysts [7][8][9][10][11], modified Fisher Tropsch catalysts over Co and Fe based catalysts modified with Ir [12][13][14][15], and alkali promoted Mo-based catalysts [16][17][18][19]. Potassium promoted MoS 2 based catalysts are a particularly promising family of catalysts [20] due to their resistance to sulfur poisoning, less severe coke deposition, and high ethanol selectivity.…”

Section: Introductionmentioning

confidence: 99%

Assessing C3–C4 alcohol synthesis pathways over a MgAl oxide supported K/MoS2 catalyst via 13C2-ethanol and 13C2-ethylene co-feeds

Claure

Lee

Goh

et al. 2016

Journal of Molecular Catalysis A: Chemical

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Mechanisms of C 3-C 4 alcohol synthesis from syngas are elucidated over a Mg/Al mixed metal oxide (MMO) supported K/MoS 2 catalyst via 13 C 2-ethanol and 13 C 2-ethylene co-feeds. K/bulk-MoS 2 is used as a control catalyst to provide insight into the role of K/MoS 2 and K/MoS 2-MMO sites on higher alcohol formation pathways. Analysis of the products via 13 C-NMR show preferential enrichment of terminal carbons in C 3-C 4 alcohols with both co-feeds, suggesting that CO insertion is the primary higher alcohol synthesis pathway, and that olefin carbonylation proceeds through the same pathway as alcohol formation. The observation of 13 C 4-1-butanol species during the CO hydrogenation reactions with 13 C 2-ethanol co-feeds provides conclusive evidence of ethanol self-coupling to 1-butanol as a secondary pathway. Additionally, acetate species are shown to be formed via an acyl precursor reacting with an alkoxy anion. Hydrogenation of an acetyl species (CH 3 CO*) to an ethoxy intermediate (C 2 H 5 O*) is shown to be largely irreversible under the reaction conditions employed, as no preferential enrichment is observed for the acetyl group in acetate species. Propionate species are shown to be formed via esterification of propionate with the corresponding alcohol, while isobutyl alcohol formation observed over both the K/bulk-MoS 2 and the MMO supported catalysts occurs via methanol coupling with 1-propanol or 1-propanol derived species.

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Cited by 36 publications

References 9 publications

Alkali-Metals on ZnO(10-10) Studied by Low-Energy Electron Diffraction and Photoelectron Spectroscopy

Alkali-Metals on ZnO(10-10) Studied by Low-Energy Electron Diffraction and Photoelectron Spectroscopy

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

Assessing C3–C4 alcohol synthesis pathways over a MgAl oxide supported K/MoS2 catalyst via 13C2-ethanol and 13C2-ethylene co-feeds

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