Gas phase acceptorless dehydrogenative coupling of ethanol over bulk MoS2 and spectroscopic measurement of structural disorder

Lauren R. McCullough; Emily S. Cheng; Abha A. Gosavi; Beata A. Kilos; David G. Barton; Eric Weitz; Harold H. Kung; Justin M. Notestein

doi:10.1016/j.jcat.2018.07.039

Gas phase acceptorless dehydrogenative coupling of ethanol over bulk MoS₂ and spectroscopic measurement of structural disorder

Lauren R. McCullough, Emily S. Cheng, Abha A. Gosavi, Beata A. Kilos, David G. Barton, Eric Weitz, Harold H. Kung, Justin M. Notestein^*

^*Corresponding author for this work

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

11 Scopus citations

Abstract

Gas phase acceptorless dehydrogenative coupling (ADC) of ethanol to ethyl acetate is investigated over bulk MoS₂. Yields of up to 56% are achieved at gas hourly space velocity of 1700 h⁻¹ and 260 °C using a high surface area co-precipitated MoS₂ material. Addition of water to the ethanol feed decreases overall conversion but increases selectivity to acetic acid. After a short activation period, the catalyst is stable over reaction times exceeding 13 h. Diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) with CO as a probe molecule and X-ray absorption spectroscopy (XAS) are used to measure structural disorder within MoS₂ samples. Samples with larger amounts of structural disorder are demonstrated to have enhanced dehydrogenation activity per total surface area.

Original language	English (US)
Pages (from-to)	159-166
Number of pages	8
Journal	Journal of Catalysis
Volume	366
DOIs	https://doi.org/10.1016/j.jcat.2018.07.039
State	Published - Oct 2018

Keywords

ADC
DRIFTS
Esters
Ethyl acetate
Metal sulfides
Molybdenum disulfide
Organic acids
Oxidation
Structural disorder
XAS

ASJC Scopus subject areas

Catalysis
Physical and Theoretical Chemistry

Access to Document

10.1016/j.jcat.2018.07.039

Cite this

@article{ed7fbcbbdd0c41a7a593d7040d216944,

title = "Gas phase acceptorless dehydrogenative coupling of ethanol over bulk MoS2 and spectroscopic measurement of structural disorder",

abstract = "Gas phase acceptorless dehydrogenative coupling (ADC) of ethanol to ethyl acetate is investigated over bulk MoS2. Yields of up to 56% are achieved at gas hourly space velocity of 1700 h−1 and 260 °C using a high surface area co-precipitated MoS2 material. Addition of water to the ethanol feed decreases overall conversion but increases selectivity to acetic acid. After a short activation period, the catalyst is stable over reaction times exceeding 13 h. Diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) with CO as a probe molecule and X-ray absorption spectroscopy (XAS) are used to measure structural disorder within MoS2 samples. Samples with larger amounts of structural disorder are demonstrated to have enhanced dehydrogenation activity per total surface area.",

keywords = "ADC, DRIFTS, Esters, Ethyl acetate, Metal sulfides, Molybdenum disulfide, Organic acids, Oxidation, Structural disorder, XAS",

author = "McCullough, {Lauren R.} and Cheng, {Emily S.} and Gosavi, {Abha A.} and Kilos, {Beata A.} and Barton, {David G.} and Eric Weitz and Kung, {Harold H.} and Notestein, {Justin M.}",

note = "Publisher Copyright: {\textcopyright} 2018 Elsevier Inc.",

year = "2018",

month = oct,

doi = "10.1016/j.jcat.2018.07.039",

language = "English (US)",

volume = "366",

pages = "159--166",

journal = "Journal of Catalysis",

issn = "0021-9517",

publisher = "Academic Press Inc.",

}

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T1 - Gas phase acceptorless dehydrogenative coupling of ethanol over bulk MoS2 and spectroscopic measurement of structural disorder

AU - McCullough, Lauren R.

AU - Cheng, Emily S.

AU - Gosavi, Abha A.

AU - Kilos, Beata A.

AU - Barton, David G.

AU - Weitz, Eric

AU - Kung, Harold H.

AU - Notestein, Justin M.

PY - 2018/10

Y1 - 2018/10

N2 - Gas phase acceptorless dehydrogenative coupling (ADC) of ethanol to ethyl acetate is investigated over bulk MoS2. Yields of up to 56% are achieved at gas hourly space velocity of 1700 h−1 and 260 °C using a high surface area co-precipitated MoS2 material. Addition of water to the ethanol feed decreases overall conversion but increases selectivity to acetic acid. After a short activation period, the catalyst is stable over reaction times exceeding 13 h. Diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) with CO as a probe molecule and X-ray absorption spectroscopy (XAS) are used to measure structural disorder within MoS2 samples. Samples with larger amounts of structural disorder are demonstrated to have enhanced dehydrogenation activity per total surface area.

AB - Gas phase acceptorless dehydrogenative coupling (ADC) of ethanol to ethyl acetate is investigated over bulk MoS2. Yields of up to 56% are achieved at gas hourly space velocity of 1700 h−1 and 260 °C using a high surface area co-precipitated MoS2 material. Addition of water to the ethanol feed decreases overall conversion but increases selectivity to acetic acid. After a short activation period, the catalyst is stable over reaction times exceeding 13 h. Diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) with CO as a probe molecule and X-ray absorption spectroscopy (XAS) are used to measure structural disorder within MoS2 samples. Samples with larger amounts of structural disorder are demonstrated to have enhanced dehydrogenation activity per total surface area.

KW - ADC

KW - DRIFTS

KW - Esters

KW - Ethyl acetate

KW - Metal sulfides

KW - Molybdenum disulfide

KW - Organic acids

KW - Oxidation

KW - Structural disorder

KW - XAS

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DO - 10.1016/j.jcat.2018.07.039

M3 - Article

AN - SCOPUS:85051783249

SN - 0021-9517

VL - 366

SP - 159

EP - 166

JO - Journal of Catalysis

JF - Journal of Catalysis

ER -