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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]

Abstract

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.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Univ. of Wisconsin-Madison, Madison, WI (United States)
Publication Date:
Research Org.:
Univ. of Wisconsin-Madison, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Contributing Org.:
Wisconsin Materials Research Science and Engineering Center and Sector 20 facilities at the Advanced Photon Source.
OSTI Identifier:
1434301
Grant/Contract Number:  
SC0014058
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 6; Journal Issue: 10; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; active site; atomic layer deposition (ALD); bimetallic catalyst; CO2 hydrogenation; control surface reactions (CSRs); interfacial sites; selective ethanol conversion to ethyl acetate

Citation Formats

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., and Dumesic, James A. 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]. United States: N. p., 2016. Web. doi:10.1021/acscatal.6b01805.
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. 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]. United States. doi:10.1021/acscatal.6b01805.
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., and Dumesic, James A. Tue . "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]". United States. doi:10.1021/acscatal.6b01805. https://www.osti.gov/servlets/purl/1434301.
@article{osti_1434301,
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]},
author = {Ro, Insoo and Liu, Yifei and Ball, Madelyn R. and Jackson, David H. K. and Chada, Joseph Paul and Sener, Canan and Kuech, Thomas F. and Madon, Rostam J. and Huber, George W. and Dumesic, James A.},
abstractNote = {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.},
doi = {10.1021/acscatal.6b01805},
journal = {ACS Catalysis},
number = 10,
volume = 6,
place = {United States},
year = {2016},
month = {9}
}

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