TY - JOUR
T1 - Stability and morphology of cerium oxide surfaces in an oxidizing environment
T2 - A first-principles investigation
AU - Fronzi, Marco
AU - Soon, Aloysius
AU - Delley, Bernard
AU - Traversa, Enrico
AU - Stampfl, Catherine
N1 - Funding Information:
The authors gratefully acknowledge support from the Australian Research Council (ARC), the Australian National Supercomputing Facility, the Australian Partnership for Advanced Computing (APAC), and the Australian Centre for Advanced Computing and Communications (ac3).
PY - 2009
Y1 - 2009
N2 - We present density functional theory investigations of the bulk properties of cerium oxides (Ce O2 and Ce2 O3) and the three low index surfaces of Ce O2, namely, (100), (110), and (111). For the surfaces, we consider various terminations including surface defects. Using the approach of "ab initio atomistic thermodynamics," we find that the most stable surface structure considered is the stoichiometric (111) surface under "oxygen-rich" conditions, while for a more reducing environment, the same (111) surface, but with subsurface oxygen vacancies, is found to be the most stable one, and for a highly reducing environment, the (111) Ce-terminated surface becomes energetically favored. Interestingly, this latter surface exhibits a significant reconstruction in that it becomes oxygen terminated and the upper layers resemble the Ce2 O3 (0001) surface. This structure could represent a precursor to the phase transition of Ce O2 to Ce2 O3.
AB - We present density functional theory investigations of the bulk properties of cerium oxides (Ce O2 and Ce2 O3) and the three low index surfaces of Ce O2, namely, (100), (110), and (111). For the surfaces, we consider various terminations including surface defects. Using the approach of "ab initio atomistic thermodynamics," we find that the most stable surface structure considered is the stoichiometric (111) surface under "oxygen-rich" conditions, while for a more reducing environment, the same (111) surface, but with subsurface oxygen vacancies, is found to be the most stable one, and for a highly reducing environment, the (111) Ce-terminated surface becomes energetically favored. Interestingly, this latter surface exhibits a significant reconstruction in that it becomes oxygen terminated and the upper layers resemble the Ce2 O3 (0001) surface. This structure could represent a precursor to the phase transition of Ce O2 to Ce2 O3.
UR - http://www.scopus.com/inward/record.url?scp=70349297049&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=70349297049&partnerID=8YFLogxK
U2 - 10.1063/1.3191784
DO - 10.1063/1.3191784
M3 - Article
AN - SCOPUS:70349297049
VL - 131
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
SN - 0021-9606
IS - 10
M1 - 104701
ER -