DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: The influence of nano-architectured CeOx supports in RhPd/CeO₂ for the catalytic ethanol steam reforming reaction

Abstract

The ethanol steam reforming (ESR) reaction has been tested over RhPd supported on polycrystalline ceria in comparison to structured supports composed of nanoshaped CeO₂ cubes and CeO₂ rods tailored towards the production of hydrogen. At 650-700 K the hydrogen yield follows the trend RhPd/CeO₂-cubes > RhPd/CeO₂ -rods > RhPd/CeO₂- polycrystalline, whereas at temperatures higher than 800 K the catalytic performance of all samples is similar and close to the thermodynamic equilibrium. The improved performance of RhPd/CeO₂-cubes and RhPd/CeO₂ -rods for ESR at low temperature is mainly ascribed to higher water-gas shift activity and a strong interaction between the bimetallic - oxide support interaction. STEM analysis shows the existence of RhPd alloyed nanoparticles in all samples, with no apparent relationship between ESR performance and RhPd particle size. X-ray diffraction under operating conditions shows metal reorganization on {100} and {110} ceria crystallographic planes during catalyst activation and ESR, but not on {111} ceria crystallographic planes. The RhPd reconstructing and tuned activation over ceria nanocubes and nanorods is considered the main reason for better catalytic activity with respect to conventional catalysts based on polycrystalline ceria

Authors:
 [1];  [2];  [1];  [2];  [3];  [1]
  1. Univ. Politècnica de Catalunya, Barcelona (Spain)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Univ. di Udine, Udine (Italy)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1188250
Alternate Identifier(s):
OSTI ID: 1251821
Report Number(s):
BNL-108064-2015-JA
Journal ID: ISSN 0920-5861; R&D Project: Co009; KC0302010
Grant/Contract Number:  
SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
Catalysis Today
Additional Journal Information:
Journal Volume: 253; Journal Issue: C; Journal ID: ISSN 0920-5861
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Divins, N. J., Senanayake, S. D., Casanovas, A., Xu, W., Trovarelli, A., and Llorca, J. The influence of nano-architectured CeOx supports in RhPd/CeO₂ for the catalytic ethanol steam reforming reaction. United States: N. p., 2015. Web. doi:10.1016/j.cattod.2014.12.042.
Divins, N. J., Senanayake, S. D., Casanovas, A., Xu, W., Trovarelli, A., & Llorca, J. The influence of nano-architectured CeOx supports in RhPd/CeO₂ for the catalytic ethanol steam reforming reaction. United States. https://doi.org/10.1016/j.cattod.2014.12.042
Divins, N. J., Senanayake, S. D., Casanovas, A., Xu, W., Trovarelli, A., and Llorca, J. Mon . "The influence of nano-architectured CeOx supports in RhPd/CeO₂ for the catalytic ethanol steam reforming reaction". United States. https://doi.org/10.1016/j.cattod.2014.12.042. https://www.osti.gov/servlets/purl/1188250.
@article{osti_1188250,
title = {The influence of nano-architectured CeOx supports in RhPd/CeO₂ for the catalytic ethanol steam reforming reaction},
author = {Divins, N. J. and Senanayake, S. D. and Casanovas, A. and Xu, W. and Trovarelli, A. and Llorca, J.},
abstractNote = {The ethanol steam reforming (ESR) reaction has been tested over RhPd supported on polycrystalline ceria in comparison to structured supports composed of nanoshaped CeO₂ cubes and CeO₂ rods tailored towards the production of hydrogen. At 650-700 K the hydrogen yield follows the trend RhPd/CeO₂-cubes > RhPd/CeO₂ -rods > RhPd/CeO₂- polycrystalline, whereas at temperatures higher than 800 K the catalytic performance of all samples is similar and close to the thermodynamic equilibrium. The improved performance of RhPd/CeO₂-cubes and RhPd/CeO₂ -rods for ESR at low temperature is mainly ascribed to higher water-gas shift activity and a strong interaction between the bimetallic - oxide support interaction. STEM analysis shows the existence of RhPd alloyed nanoparticles in all samples, with no apparent relationship between ESR performance and RhPd particle size. X-ray diffraction under operating conditions shows metal reorganization on {100} and {110} ceria crystallographic planes during catalyst activation and ESR, but not on {111} ceria crystallographic planes. The RhPd reconstructing and tuned activation over ceria nanocubes and nanorods is considered the main reason for better catalytic activity with respect to conventional catalysts based on polycrystalline ceria},
doi = {10.1016/j.cattod.2014.12.042},
journal = {Catalysis Today},
number = C,
volume = 253,
place = {United States},
year = {Mon Jan 19 00:00:00 EST 2015},
month = {Mon Jan 19 00:00:00 EST 2015}
}

Journal Article:

Citation Metrics:
Cited by: 40 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Size dependent optical properties of LaB6 nanoparticles enhanced by localized surface plasmon resonance
journal, November 2013


CeO 2 Nanorods and Gold Nanocrystals Supported on CeO 2 Nanorods as Catalyst
journal, October 2005

  • Huang, P. X.; Wu, F.; Zhu, B. L.
  • The Journal of Physical Chemistry B, Vol. 109, Issue 41
  • DOI: 10.1021/jp052978u

Morphology Dependence of Catalytic Properties of Ni/CeO 2 Nanostructures for Carbon Dioxide Reforming of Methane
journal, April 2012

  • Du, Xianjun; Zhang, Dengsong; Shi, Liyi
  • The Journal of Physical Chemistry C, Vol. 116, Issue 18
  • DOI: 10.1021/jp300543r

Pt/CeO2 catalysts in crotonaldehyde hydrogenation: Selectivity, metal particle size and SMSI states
journal, January 2006

  • Abid, Mohamed; Paul-Boncour, Valerie; Touroude, Raymonde
  • Applied Catalysis A: General, Vol. 297, Issue 1
  • DOI: 10.1016/j.apcata.2005.08.048

Hydrogen Production from Ethanol over Rh–Pd/CeO2 Catalysts
journal, October 2008


Surface-structure sensitivity of CO oxidation over polycrystalline ceria powders
journal, August 2005


Shape and Crystal-Plane Effects of Nanoscale Ceria on the Activity of Au-CeO2 Catalysts for the Water–Gas Shift Reaction
journal, March 2008

  • Si, Rui; Flytzani-Stephanopoulos, Maria
  • Angewandte Chemie International Edition, Vol. 47, Issue 15, p. 2884-2887
  • DOI: 10.1002/anie.200705828

Steam and auto-thermal reforming of bio-ethanol over MgO and CeO2CeO2 Ni supported catalysts
journal, December 2006


Time-resolved Studies for the Mechanism of Reduction of Copper Oxides with Carbon Monoxide:  Complex Behavior of Lattice Oxygen and the Formation of Suboxides
journal, September 2004

  • Wang, Xianqin; Hanson, Jonathan C.; Frenkel, Anatoly I.
  • The Journal of Physical Chemistry B, Vol. 108, Issue 36
  • DOI: 10.1021/jp040366o

Steam reforming of methanol over ceria and gold-ceria nanoshapes
journal, March 2010


Influence of the support on surface rearrangements of bimetallic nanoparticles in real catalysts
journal, October 2014


Synthesis of porous CuO–CeO2 nanospheres with an enhanced low-temperature CO oxidation activity
journal, January 2010

  • Qin, Jinwen; Lu, Junfeng; Cao, Minhua
  • Nanoscale, Vol. 2, Issue 12
  • DOI: 10.1039/c0nr00446d

Ethanol steam reforming over Co/CeO2 catalysts: Investigation of the effect of ceria morphology
journal, December 2012


New insight into mechanisms in water-gas-shift reaction on Au/CeO2(111): A density functional theory and kinetic study
journal, January 2011

  • Chen, Ying; Wang, Haifeng; Burch, Robbie
  • Faraday Discussions, Vol. 152
  • DOI: 10.1039/c1fd00019e

Active gold species on cerium oxide nanoshapes for methanol steam reforming and the water gas shift reactions
journal, January 2010

  • Yi, Nan; Si, Rui; Saltsburg, Howard
  • Energy & Environmental Science, Vol. 3, Issue 6
  • DOI: 10.1039/b924051a

The role of cationic Au3+ and nonionic Au0 species in the low-temperature water–gas shift reaction on Au/CeO2 catalysts
journal, December 2007


The effect of the morphology of nanocrystalline CeO2 on ethanol reforming
journal, June 2007


A Phenomenological Study of the Metal-Oxide Interface: The Role of Catalysis in Hydrogen Production from Renewable Resources
journal, November 2008


Shape-controlled synthesis and catalytic application of ceria nanomaterials
journal, January 2012

  • Zhang, Dengsong; Du, Xianjun; Shi, Liyi
  • Dalton Transactions, Vol. 41, Issue 48
  • DOI: 10.1039/c2dt31759a

Bio-ethanol steam reforming and autothermal reforming in 3-μm channels coated with RhPd/CeO2 for hydrogen generation
journal, February 2013

  • Divins, Núria J.; López, Eduardo; Rodríguez, Ángel
  • Chemical Engineering and Processing: Process Intensification, Vol. 64
  • DOI: 10.1016/j.cep.2012.10.018

Effect of higher alcohols on the performances of a 1%Rh/MgAl2O4/Al2O3 catalyst for hydrogen production by crude bioethanol steam reforming
journal, January 2011


Morphology and Crystal-Plane Effects of Nanoscale Ceria on the Activity of CuO/CeO2 for NO Reduction by CO
journal, April 2011


Great Influence of Anions for Controllable Synthesis of CeO 2 Nanostructures: From Nanorods to Nanocubes
journal, October 2008

  • Wu, Qiang; Zhang, Fan; Xiao, Pei
  • The Journal of Physical Chemistry C, Vol. 112, Issue 44
  • DOI: 10.1021/jp804140e

Morphology effects of nanoscale ceria on the activity of Au/CeO2 catalysts for low-temperature CO oxidation
journal, July 2009


High-Throughput Continuous Hydrothermal Synthesis of an Entire Nanoceramic Phase Diagram
journal, September 2009

  • Weng, Xiaole; Cockcroft, Jeremy K.; Hyett, Geoffrey
  • Journal of Combinatorial Chemistry, Vol. 11, Issue 5
  • DOI: 10.1021/cc900041a

Surface-dependent oxidation of H 2 on CeO 2 surfaces
journal, January 2013


Opposite Face Sensitivity of CeO 2 in Hydrogenation and Oxidation Catalysis
journal, August 2014

  • Vilé, Gianvito; Colussi, Sara; Krumeich, Frank
  • Angewandte Chemie International Edition, Vol. 53, Issue 45
  • DOI: 10.1002/anie.201406637

Hydrogen production from ethanol over Pd–Rh/CeO2 with a metallic membrane reactor
journal, October 2012


Configurational lattice dynamics: The phase diagram of Rh Pd
journal, April 2005


Probing Defect Sites on CeO 2 Nanocrystals with Well-Defined Surface Planes by Raman Spectroscopy and O 2 Adsorption
journal, November 2010

  • Wu, Zili; Li, Meijun; Howe, Jane
  • Langmuir, Vol. 26, Issue 21
  • DOI: 10.1021/la101723w

Oxygen Vacancy Clusters Promoting Reducibility and Activity of Ceria Nanorods
journal, March 2009

  • Liu, Xiangwen; Zhou, Kebin; Wang, Lei
  • Journal of the American Chemical Society, Vol. 131, Issue 9
  • DOI: 10.1021/ja808433d

Design of Nanocatalysts for Green Hydrogen Production from Bioethanol
journal, December 2011


Ethanol catalytic membrane reformer for direct PEM FC feeding
journal, May 2013


Shape-Dependent Activity of Ceria in Soot Combustion
journal, December 2013

  • Aneggi, Eleonora; Wiater, Dawid; de Leitenburg, Carla
  • ACS Catalysis, Vol. 4, Issue 1
  • DOI: 10.1021/cs400850r

Cobalt hydrotalcites as catalysts for bioethanol steam reforming. The promoting effect of potassium on catalyst activity and long-term stability
journal, October 2012


Works referencing / citing this record:

Effects of preparation mode and doping on the genesis and properties of Ni/Ce1-xMxOy nanocrystallites (M = Gd, La, Mg) for catalytic applications
journal, January 2019

  • Matus, Ekaterina V.; Okhlopkova, Lyudmila B.; Sukhova, Olga B.
  • Journal of Nanoparticle Research, Vol. 21, Issue 1
  • DOI: 10.1007/s11051-018-4454-5