Role of the Cu-ZrO2 Interfacial Sites for Conversion of Ethanol to Ethyl Acetate and Synthesis of Methanol from CO2 and H2 [The Role of the Cu-ZrO2 Interfacial Sites for Ethanol Conversion to Ethyl Acetate and Methanol Synthesis from CO2 and H2]

Ro, Insoo; Liu, Yifei; Ball, Madelyn R.; Jackson, David H. K.; Chada, Joseph Paul; Sener, Canan; Kuech, Thomas F.; Madon, Rostam J.; Huber, George W.; Dumesic, James A.

doi:10.1021/acscatal.6b01805

Title: Role of the Cu-ZrO₂ Interfacial Sites for Conversion of Ethanol to Ethyl Acetate and Synthesis of Methanol from CO₂ and H₂ [The Role of the Cu-ZrO₂ Interfacial Sites for Ethanol Conversion to Ethyl Acetate and Methanol Synthesis from CO₂ and H₂]

Journal Article · Tue Sep 06 00:00:00 EDT 2016 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.6b01805· OSTI ID:1434301

Ro, Insoo ^[1]; Liu, Yifei ^[1]; Ball, Madelyn R. ^[1]; Jackson, David H. K. ^[1]; Chada, Joseph Paul ^[1]; Sener, Canan ^[1]; Kuech, Thomas F. ^[1]; Madon, Rostam J. ^[1]; Huber, George W. ^[1]; Dumesic, James A. ^[1]

Univ. of Wisconsin-Madison, Madison, WI (United States)

Well-defined Cu catalysts containing different amounts of zirconia were synthesized by controlled surface reactions (CSRs) and atomic layer deposition methods and studied for the selective conversion of ethanol to ethyl acetate and for methanol synthesis. Selective deposition of ZrO₂ on undercoordinated Cu sites or near Cu nanoparticles via the CSR method was evidenced by UV–vis absorption spectroscopy, scanning transmission electron microscopy, and inductively coupled plasma absorption emission spectroscopy. The concentrations of Cu and Cu-ZrO₂ interfacial sites were quantified using a combination of subambient CO Fourier transform infrared spectroscopy and reactive N₂O chemisorption measurements. The oxidation states of the Cu and ZrO₂ species for these catalysts were determined using X-ray absorption near edge structure measurements, showing that these species were present primarily as Cu⁰ and Zr⁴⁺, respectively. Here, it was found that the formation of Cu-ZrO₂ interfacial sites increased the turnover frequency by an order of magnitude in both the conversion of ethanol to ethyl acetate and the synthesis of methanol from CO₂ and H₂.

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Research Organization:: Univ. of Wisconsin, Madison, WI (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Contributing Organization:: Wisconsin Materials Research Science and Engineering Center and Sector 20 facilities at the Advanced Photon Source.

Grant/Contract Number:: SC0014058

OSTI ID:: 1434301

Journal Information:: ACS Catalysis, Vol. 6, Issue 10; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 120 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
active site
atomic layer deposition (ALD)
bimetallic catalyst
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control surface reactions (CSRs)
interfacial sites
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Title: Role of the Cu-ZrO2 Interfacial Sites for Conversion of Ethanol to Ethyl Acetate and Synthesis of Methanol from CO2 and H2 [The Role of the Cu-ZrO2 Interfacial Sites for Ethanol Conversion to Ethyl Acetate and Methanol Synthesis from CO2 and H2]

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Title: Role of the Cu-ZrO₂ Interfacial Sites for Conversion of Ethanol to Ethyl Acetate and Synthesis of Methanol from CO₂ and H₂ [The Role of the Cu-ZrO₂ Interfacial Sites for Ethanol Conversion to Ethyl Acetate and Methanol Synthesis from CO₂ and H₂]