Role of surface defects in activation of O2 and N2O on ZrO2 and yttrium-stabilized ZrO2.

Share/Save/Bookmark

Zhu, Jianjun and Albertsma, Sander and Ommen van, Jan G. and Lefferts, Leon (2005) Role of surface defects in activation of O2 and N2O on ZrO2 and yttrium-stabilized ZrO2. Journal of Physical Chemistry B: Materials, surfaces, interfaces, & biophysical, 109 (19). pp. 9550-9555. ISSN 1520-6106

[img]PDF
Restricted to UT campus only
: Request a copy
270Kb
Abstract:The relationship between the structure of both yttrium-stabilized zirconia (YSZ) and ZrO2 catalysts and their ability to activate N2O and O2 is studied by determination of catalytic properties and characterization with TPD, SEM, and XRD. Furthermore, the role of oxygen species formed via dissociation of either O2 or N2O in catalytic partial oxidation of methane (CPOM) is determined. N2O can be activated at both structural defects (e.g., Zr cations located at corners) and intrinsic oxygen vacancies (--) and forms two types of oxygen species (-O and -O) on the surface, respectively. In contrast, molecular oxygen gives rise to only one type of oxygen species (-O), that is, surface lattice oxygen. This type of oxygen species can be extracted by reaction with methane, forming the intrinsic oxygen vacancies again during CPOM. However, the structural defects are not active for oxygen activation during CPOM. Doping ZrO2 with Y2O3 significantly decreases the number of structural defects via replacement of Zr4+ cations by Y3+ cations, located at corners, steps, kinks, and edges of the crystallites. Calcination at higher temperatures results in less structural defects due to both increasing crystallite size as well as transformation to more regular shaped crystallites. High temperature calcinations also increase the activity of YSZ in CPOM. This is attributed to the increase in the exposition of low index planes, especially those (111) with the lowest surface energy and the highest coordination numbers, induced by the thermal treatment
Item Type:Article
Copyright:© 2005 American Chemical Society
Faculty:
Science and Technology (TNW)
Research Group:
Link to this item:http://purl.utwente.nl/publications/54139
Official URL:http://dx.doi.org/10.1021/jp050258h
Export this item as:BibTeX
EndNote
HTML Citation
Reference Manager

 

Repository Staff Only: item control page

Metis ID: 227830