skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Energy efficient microwave synthesis of mesoporous Ce0.5M0.5O2 (Ti, Zr, Hf) nanoparticles for low temperature CO oxidation in an ionic liquid – a comparative study

Abstract

Ce0.5M0.5O2 (M = Ti, Zr, Hf) nanoparticles have been successfully synthesized by microwave irradiation in the ionic liquid [C4mim][Tf2N] (1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)amide). The morphology, crystallinity, and chemical composition of the obtained materials were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDX), Raman spectroscopy, and N2–adsorption measurements. XRD and Raman spectroscopy analyses confirmed the formation of solid solutions with cubic fluorite structure. The catalytic activities of the Ce0.5M0.5O2 (M = Ti, Zr, Hf) nanoparticles were investigated in the low-temperature oxidation of CO. Ce0.5Zr0.5O2 nanospheres exhibit the best performance (100% conversion at 350 °C), followed by Ce0.5Hf0.5O2 (55% conversion at 360 °C) and Ce0.5Ti0.5O2 (11% conversion at 350 °C). Heating the as-prepared Ce0.5Zr0.5O2 to 600 °C for extended time leads to a decrease in surface area and, as expected decreased catalytic activity. Depending on the ionic liquid the obtained Ce0.5Zr0.5O2 exhibits different morphologies, varying from nano-spheres in [C4mim][Tf2N] and [P66614][Tf2N] (P66614 = trishexyltetradecylphosphonium) to sheet-like assemblies in [C3mimOH][Tf2N] (C3mimOH = 1-(3-hydroxypropyl)-3-methylimidazolium). As a result, the microwave synthesis superiority to other heating methods like sonochemical synthesis and conventional heating was proven by comparative experiments where the catalytic activity of Ce0.5Zr0.5O2 obtained by alternate methods such as conventional heatingmore » was found to be poorer than that of the microwave-synthesised material.« less

Authors:
 [1];  [2];  [3]
  1. Ruhr-Univ. Bochum, Bochum (Germany)
  2. Ruhr-Univ. Bochum, Bochum (Germany); Cardiff Univ., Wales (United Kingdom)
  3. Ruhr-Univ. Bochum, Bochum (Germany); Ames Lab., Ames, IA (United States)
Publication Date:
Research Org.:
Ames Lab., Ames, IA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1239143
Report Number(s):
IS-J-8628
Journal ID: ISSN 1144-0546; NJCHE5
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
New Journal of Chemistry
Additional Journal Information:
Journal Volume: 39; Journal Issue: 2; Journal ID: ISSN 1144-0546
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Alammar, Tarek, Chow, Ying -Kit, and Mudring, Anja -Verena. Energy efficient microwave synthesis of mesoporous Ce0.5M0.5O2 (Ti, Zr, Hf) nanoparticles for low temperature CO oxidation in an ionic liquid – a comparative study. United States: N. p., 2014. Web. https://doi.org/10.1039/c4nj00951g.
Alammar, Tarek, Chow, Ying -Kit, & Mudring, Anja -Verena. Energy efficient microwave synthesis of mesoporous Ce0.5M0.5O2 (Ti, Zr, Hf) nanoparticles for low temperature CO oxidation in an ionic liquid – a comparative study. United States. https://doi.org/10.1039/c4nj00951g
Alammar, Tarek, Chow, Ying -Kit, and Mudring, Anja -Verena. Wed . "Energy efficient microwave synthesis of mesoporous Ce0.5M0.5O2 (Ti, Zr, Hf) nanoparticles for low temperature CO oxidation in an ionic liquid – a comparative study". United States. https://doi.org/10.1039/c4nj00951g. https://www.osti.gov/servlets/purl/1239143.
@article{osti_1239143,
title = {Energy efficient microwave synthesis of mesoporous Ce0.5M0.5O2 (Ti, Zr, Hf) nanoparticles for low temperature CO oxidation in an ionic liquid – a comparative study},
author = {Alammar, Tarek and Chow, Ying -Kit and Mudring, Anja -Verena},
abstractNote = {Ce0.5M0.5O2 (M = Ti, Zr, Hf) nanoparticles have been successfully synthesized by microwave irradiation in the ionic liquid [C4mim][Tf2N] (1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)amide). The morphology, crystallinity, and chemical composition of the obtained materials were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDX), Raman spectroscopy, and N2–adsorption measurements. XRD and Raman spectroscopy analyses confirmed the formation of solid solutions with cubic fluorite structure. The catalytic activities of the Ce0.5M0.5O2 (M = Ti, Zr, Hf) nanoparticles were investigated in the low-temperature oxidation of CO. Ce0.5Zr0.5O2 nanospheres exhibit the best performance (100% conversion at 350 °C), followed by Ce0.5Hf0.5O2 (55% conversion at 360 °C) and Ce0.5Ti0.5O2 (11% conversion at 350 °C). Heating the as-prepared Ce0.5Zr0.5O2 to 600 °C for extended time leads to a decrease in surface area and, as expected decreased catalytic activity. Depending on the ionic liquid the obtained Ce0.5Zr0.5O2 exhibits different morphologies, varying from nano-spheres in [C4mim][Tf2N] and [P66614][Tf2N] (P66614 = trishexyltetradecylphosphonium) to sheet-like assemblies in [C3mimOH][Tf2N] (C3mimOH = 1-(3-hydroxypropyl)-3-methylimidazolium). As a result, the microwave synthesis superiority to other heating methods like sonochemical synthesis and conventional heating was proven by comparative experiments where the catalytic activity of Ce0.5Zr0.5O2 obtained by alternate methods such as conventional heating was found to be poorer than that of the microwave-synthesised material.},
doi = {10.1039/c4nj00951g},
journal = {New Journal of Chemistry},
number = 2,
volume = 39,
place = {United States},
year = {2014},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 9 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Oxygen vacancy formation and migration in Ce1−xZrxO2 catalyst: A DFT+U calculation
journal, June 2010

  • Chen, Hsin-Tsung; Chang, Jee-Gong
  • The Journal of Chemical Physics, Vol. 132, Issue 21
  • DOI: 10.1063/1.3429314

Size dependency variation in lattice parameter and valency states in nanocrystalline cerium oxide
journal, September 2005

  • Deshpande, Sameer; Patil, Swanand; Kuchibhatla, Satyanarayana VNT
  • Applied Physics Letters, Vol. 87, Issue 13
  • DOI: 10.1063/1.2061873

Greatly facilitated oxygen vacancy formation in ceria nanocrystallites
journal, January 2010

  • Migani, Annapaola; Vayssilov, Georgi N.; Bromley, Stefan T.
  • Chemical Communications, Vol. 46, Issue 32
  • DOI: 10.1039/c0cc01091j

Study of nano-structured ceria for catalytic CO oxidation
journal, January 2011

  • Valechha, Dolly; Lokhande, Suchita; Klementova, Mariana
  • Journal of Materials Chemistry, Vol. 21, Issue 11
  • DOI: 10.1039/c0jm03267k

Microwave assisted organic synthesis—a review
journal, November 2001


Continuous Flow Hydroformylation of Alkenes in Supercritical Fluid−Ionic Liquid Biphasic Systems
journal, December 2003

  • Webb, Paul B.; Sellin, Murielle F.; Kunene, Thulani E.
  • Journal of the American Chemical Society, Vol. 125, Issue 50
  • DOI: 10.1021/ja035967s

Ionic Liquid-Assisted Sonochemical Preparation of CeO 2 Nanoparticles for CO Oxidation
journal, December 2014

  • Alammar, Tarek; Noei, Heshmat; Wang, Yuemin
  • ACS Sustainable Chemistry & Engineering, Vol. 3, Issue 1
  • DOI: 10.1021/sc500387k

Low-temperature route to metal titanate perovskite nanoparticles for photocatalytic applications
journal, November 2015


Facile ultrasound-assisted synthesis of ZnO nanorods in an ionic liquid
journal, April 2009


Facile preparation of Ag/ZnO nanoparticles via photoreduction
journal, June 2009


Sonochemical preparation of TiO2 nanoparticles in the ionic liquid 1-(3-hydroxypropyl)-3-methylimidazolium-bis(trifluoromethylsulfonyl)amide
journal, March 2010


Ultrasound-Assisted Synthesis of CuO Nanorods in a Neat Room-Temperature Ionic Liquid
journal, July 2009

  • Alammar, Tarek; Birkner, Alexander; Mudring, Anja-Verena
  • European Journal of Inorganic Chemistry, Vol. 2009, Issue 19
  • DOI: 10.1002/ejic.200900093

Surface chemistry and microstructural analysis of CexZr1−xO2−y model catalyst surfaces
journal, April 2003


Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976


Thermodynamic Investigation of the Redox Properties for Ceria−Hafnia, Ceria−Terbia, and Ceria−Praseodymia Solid Solutions
journal, August 2008

  • Zhou, Gong; Gorte, Raymond J.
  • The Journal of Physical Chemistry B, Vol. 112, Issue 32
  • DOI: 10.1021/jp804089w

Oxidation entropies and enthalpies of ceria–zirconia solid solutions
journal, May 2007


A surfactant and template-free route for synthesizing ceria nanocrystals with tunable morphologies
journal, January 2010

  • Wang, Wei; Howe, Jane Y.; Li, Yuan
  • Journal of Materials Chemistry, Vol. 20, Issue 36
  • DOI: 10.1039/c0jm00982b

Synthesis, characterization and photoluminescence of CeO2 nanoparticles by a facile method at room temperature
journal, March 2010


Synthesis of Nanosized Ceria-Zirconia Solid Solutions by a Rapid Microwave-Assisted Combustion Method
journal, June 2009

  • Reddy, Benjaram M.; Reddy, Gunugunuri K.; Reddy, Lankela H.
  • The Open Physical Chemistry Journal, Vol. 3, Issue 1
  • DOI: 10.2174/1874067700903010024

Sol–gel synthesis and phase composition of ultrafine ceria-doped zirconia powders for functional ceramics
journal, July 2012


A novel and simple route to catalysts with a high oxygen storage capacity: the direct room-temperature synthesis of CeO 2 –ZrO 2 solid solutions
journal, January 1995

  • de Leitenburg, Carla; Trovarelli, Alessandro; Zamar, Francesca
  • J. Chem. Soc., Chem. Commun., Issue 21
  • DOI: 10.1039/C39950002181

Sonohydrothermal Synthesis of Nanostructured (Ce,Zr)O 2 Mixed Oxides with Enhanced Catalytic Performance
journal, October 2013

  • Cau, Camille; Guari, Yannick; Chave, Tony
  • The Journal of Physical Chemistry C, Vol. 117, Issue 44
  • DOI: 10.1021/jp407096p

The role of oxygen vacancies on ceria surfaces in the oxidation of carbon monoxide
journal, September 1994


Synthesis of LaMnO3+δby Firing Gels Using Citric Acid
journal, February 1997

  • Taguchi, Hideki; Matsu-ura, Shin-ichiro; Nagao, Mahiko
  • Journal of Solid State Chemistry, Vol. 129, Issue 1
  • DOI: 10.1006/jssc.1996.7229

Tuning the internal structures of CdSeS nanoparticles by using different selenium and sulphur precursors
journal, January 2010

  • Chen, Xianfeng; Hutchison, John L.; Dobson, Peter J.
  • Materials Science and Engineering: B, Vol. 166, Issue 1
  • DOI: 10.1016/j.mseb.2009.09.021

General and facile synthesis of ceria-based solid solution nanocrystals and their catalytic properties
journal, September 2009


Sonochemical Synthesis of 0D, 1D, and 2D Zinc Oxide Nanostructures in Ionic Liquids and Their Photocatalytic Activity
journal, December 2011


Mild yet phase-selective preparation of TiO2 nanoparticles from ionic liquids – a critical study
journal, January 2013

  • Alammar, Tarek; Noei, Heshmat; Wang, Yuemin
  • Nanoscale, Vol. 5, Issue 17
  • DOI: 10.1039/c3nr00824j

Ultrasound-assisted synthesis of mesoporous β-Ni(OH)2 and NiO nano-sheets using ionic liquids
journal, January 2012

  • Alammar, Tarek; Shekhah, Osama; Wohlgemuth, Jonas
  • Journal of Materials Chemistry, Vol. 22, Issue 35
  • DOI: 10.1039/c2jm32849f

Surface-Enhanced Vibrational Spectroscopy of Tetrafluoroborate 1- n -Butyl-3-methylimidazolium (BMIBF 4 ) Ionic Liquid on Silver Surfaces
journal, November 2008

  • Rubim, Joel C.; Trindade, Flavio A.; Gelesky, Marcos A.
  • The Journal of Physical Chemistry C, Vol. 112, Issue 49
  • DOI: 10.1021/jp808101g

Disclosure of the imidazolium cation coordination and stabilization mode in ionic liquid stabilized gold(0) nanoparticles
journal, December 2007

  • Schrekker, Henri S.; Gelesky, Marcos A.; Stracke, Marcelo P.
  • Journal of Colloid and Interface Science, Vol. 316, Issue 1
  • DOI: 10.1016/j.jcis.2007.08.018

The role of charge-enhanced C–H⋯O interactions in gel-like mixtures prepared from ionic liquids and tungsten(VI) oxide nanoparticles
journal, August 2006


Microwave synthesis and inherent stabilization of metal nanoparticles in 1-methyl-3-(3-carboxyethyl)-imidazolium tetrafluoroborate
journal, January 2011

  • Marquardt, Dorothea; Xie, Zailai; Taubert, Andreas
  • Dalton Transactions, Vol. 40, Issue 33
  • DOI: 10.1039/c1dt10795j

Synthesis and characterization of nickel nanoparticles dispersed in imidazolium ionic liquids
journal, January 2007

  • Migowski, Pedro; Machado, Giovanna; Texeira, Sergio R.
  • Physical Chemistry Chemical Physics, Vol. 9, Issue 34
  • DOI: 10.1039/b703979d

Density and viscosity of several pure and water-saturated ionic liquids
journal, January 2006

  • Jacquemin, J.; Husson, P.; Padua, A. A. H.
  • Green Chem., Vol. 8, Issue 2
  • DOI: 10.1039/B513231B

Eu3+ as a dual probe for the determination of IL anion donor power: A combined luminescence spectroscopic and electrochemical approach
journal, April 2014


Structural and Electrochemical Properties of YbIII in Various Ionic Liquids
journal, September 2010

  • Babai, Arash; Pitula, Slawomir; Mudring, Anja-Verena
  • European Journal of Inorganic Chemistry, Vol. 2010, Issue 31
  • DOI: 10.1002/ejic.201000323

Synthesis, Structure, and Physico-optical Properties of Manganate(II)-Based Ionic Liquids
journal, March 2010

  • Pitula, Slawomir; Mudring, Anja-Verena
  • Chemistry - A European Journal, Vol. 16, Issue 11
  • DOI: 10.1002/chem.200802660

Optical basicity of ionic liquids
journal, January 2010

  • Pitula, Slawomir; Mudring, Anja-Verena
  • Physical Chemistry Chemical Physics, Vol. 12, Issue 26
  • DOI: 10.1039/b925606g

[Ni(tmen)(acac)][B(Ph)4] a probe for the anion basicity of ionic liquids
journal, January 2010

  • Bartosik, Joanna; Mudring, Anja-Verena
  • Physical Chemistry Chemical Physics, Vol. 12, Issue 16
  • DOI: 10.1039/b920530f

Microwave hydrothermal synthesis of MSnO3 (M2+ = Ca2+, Sr2+, Ba2+): effect of M2+ on crystal structure and photocatalytic properties
journal, December 2013


    Works referencing / citing this record:

    Pentagonal Bismuth Antiprisms with Endohedral Palladium or Platinum Atoms by Low-Temperature Syntheses: Pentagonal Bismuth Antiprisms with Endohedral Palladium or Platinum Atoms by Low-Temperature Syntheses
    journal, November 2016

    • Groh, Matthias F.; Wolff, Alexander; Wahl, Bernhard
    • Zeitschrift für anorganische und allgemeine Chemie, Vol. 643, Issue 1
    • DOI: 10.1002/zaac.201600354

    The Intermetalloid Clusters [Ni 2 Bi 12 ] 4+ and [Rh 2 Bi 12 ] 4+ - Ionothermal Synthesis, Crystal Structures, and Chemical Bonding : The Intermetalloid Clusters [Ni
    journal, November 2018

    • Groh, Matthias F.; Müller, Ulrike; Isaeva, Anna
    • Zeitschrift für anorganische und allgemeine Chemie, Vol. 645, Issue 3
    • DOI: 10.1002/zaac.201800441

    Cr-Doped CeO2 Nanorods for CO Oxidation: Insights into Promotional Effect of Cr on Structure and Catalytic Performance
    journal, November 2019


    Synthesis and Dissolution of Metal Oxides in Ionic Liquids and Deep Eutectic Solvents
    journal, December 2019