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Title: Dry reforming of methane on a highly-active Ni-CeO 2 catalyst: Effects of metal-support interactions on C–H bond breaking

Abstract

Ni-CeO 2 is a highly efficient, stable and non-expensive catalyst for methane dry reforming at relative low temperatures (700 K). The active phase of the catalyst consists of small nanoparticles of nickel dispersed on partially reduced ceria. Experiments of ambient pressure XPS indicate that methane dissociates on Ni/CeO 2 at temperatures as low as 300 K, generating CH x and CO x species on the surface of the catalyst. Strong metal–support interactions activate Ni for the dissociation of methane. The results of density-functional calculations show a drop in the effective barrier for methane activation from 0.9 eV on Ni(111) to only 0.15 eV on Ni/CeO 2–x(111). At 700 K, under methane dry reforming conditions, no signals for adsorbed CH x or C species are detected in the C1s XPS region. As a result, the reforming of methane proceeds in a clean and efficient way.

Authors:
 [1];  [2];  [3];  [2];  [4];  [1];  [2];  [5];  [2];  [4];  [6];  [3];  [7];  [2];  [8]
  1. State Univ. of New York at Stony Brook, Stony Brook, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. CONICET-Univ. Nacional de Rosario (Argentina)
  4. Univ. of Wyoming, Laramie, WY (United States)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  6. CIC Energigune, Alava (Spain)
  7. Instituto de Catalisis y Petroleoquimica, CSIC, Madrid (Spain)
  8. State Univ. of New York at Stony Brook, Stony Brook NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1333199
Alternate Identifier(s):
OSTI ID: 1378983; OSTI ID: 1400562
Report Number(s):
BNL-113195-2016-JA
Journal ID: ISSN 1433-7851; R&D Project: CO040; KC0302010
Grant/Contract Number:  
SC0012704; AC02-05CH11231; CTQ2012-32928; CTQ2015-71823-R
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 55; Journal Issue: 26; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; nickel; ceria; methane dissociation; X-ray photoelectron spectroscopy; density functional theory

Citation Formats

Liu, Zongyuan, Grinter, David C., Lustemberg, Pablo G., Nguyen-Phan, Thuy -Duong, Zhou, Yinghui, Luo, B. Sc. Si, Waluyo, Iradwikanari, Crumlin, Ethan J., Stacchiola, Dario J., Zhou, Jing, Carrasco, Javier, Busnengo, H. Fabio, Ganduglia-Pirovano, M. Verónica, Senanayake, Sanjaya D., and Rodriguez, Jose A. Dry reforming of methane on a highly-active Ni-CeO2 catalyst: Effects of metal-support interactions on C–H bond breaking. United States: N. p., 2016. Web. doi:10.1002/anie.201602489.
Liu, Zongyuan, Grinter, David C., Lustemberg, Pablo G., Nguyen-Phan, Thuy -Duong, Zhou, Yinghui, Luo, B. Sc. Si, Waluyo, Iradwikanari, Crumlin, Ethan J., Stacchiola, Dario J., Zhou, Jing, Carrasco, Javier, Busnengo, H. Fabio, Ganduglia-Pirovano, M. Verónica, Senanayake, Sanjaya D., & Rodriguez, Jose A. Dry reforming of methane on a highly-active Ni-CeO2 catalyst: Effects of metal-support interactions on C–H bond breaking. United States. doi:10.1002/anie.201602489.
Liu, Zongyuan, Grinter, David C., Lustemberg, Pablo G., Nguyen-Phan, Thuy -Duong, Zhou, Yinghui, Luo, B. Sc. Si, Waluyo, Iradwikanari, Crumlin, Ethan J., Stacchiola, Dario J., Zhou, Jing, Carrasco, Javier, Busnengo, H. Fabio, Ganduglia-Pirovano, M. Verónica, Senanayake, Sanjaya D., and Rodriguez, Jose A. Wed . "Dry reforming of methane on a highly-active Ni-CeO2 catalyst: Effects of metal-support interactions on C–H bond breaking". United States. doi:10.1002/anie.201602489. https://www.osti.gov/servlets/purl/1333199.
@article{osti_1333199,
title = {Dry reforming of methane on a highly-active Ni-CeO2 catalyst: Effects of metal-support interactions on C–H bond breaking},
author = {Liu, Zongyuan and Grinter, David C. and Lustemberg, Pablo G. and Nguyen-Phan, Thuy -Duong and Zhou, Yinghui and Luo, B. Sc. Si and Waluyo, Iradwikanari and Crumlin, Ethan J. and Stacchiola, Dario J. and Zhou, Jing and Carrasco, Javier and Busnengo, H. Fabio and Ganduglia-Pirovano, M. Verónica and Senanayake, Sanjaya D. and Rodriguez, Jose A.},
abstractNote = {Ni-CeO2 is a highly efficient, stable and non-expensive catalyst for methane dry reforming at relative low temperatures (700 K). The active phase of the catalyst consists of small nanoparticles of nickel dispersed on partially reduced ceria. Experiments of ambient pressure XPS indicate that methane dissociates on Ni/CeO2 at temperatures as low as 300 K, generating CHx and COx species on the surface of the catalyst. Strong metal–support interactions activate Ni for the dissociation of methane. The results of density-functional calculations show a drop in the effective barrier for methane activation from 0.9 eV on Ni(111) to only 0.15 eV on Ni/CeO2–x(111). At 700 K, under methane dry reforming conditions, no signals for adsorbed CHx or C species are detected in the C1s XPS region. As a result, the reforming of methane proceeds in a clean and efficient way.},
doi = {10.1002/anie.201602489},
journal = {Angewandte Chemie (International Edition)},
number = 26,
volume = 55,
place = {United States},
year = {2016},
month = {5}
}

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    Works referencing / citing this record:

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