Abstract
High-throughput Screening of New Materials for Water Splitting Applications
Ivano Castelli
Technical University of Denmark
Design new materials for energy production in a photoelectrochemical
cell, where water is split into hydrogen and oxygen by solar light, is
one possible solution to the problem of increasing energy demand and
storage. A screening procedure based on ab-initio density
functional theory calculations has been applied to guide the search
for new materials. The main descriptors of the properties relevant for
the screening are: heat of formation, electronic bandgap, and
positions of the band edges with respect to the red-ox levels of
water. A recently implemented exchange-correlation functional, called
GLLB-SC [1], has been used for the estimation of the bandgaps.
Firstly, a screening procedure has been applied to 19000 cubic
perovskite structures. These are obtained by combining 52 metals
together with oxygen, nitrogen, sulfur and fluorine as anions. 32
promising materials have been found for visible light harvesting, 20
for the one-photon and 12 for the two-photon water splitting
process. In addition, 16 candidates were suggested for the
transparent shielding of the photocatalyst. The problem of corrosion
has been addressed for the candidates for the one-photon scheme using
Pourbaix diagrams [4].
Secondly, the screening has been extended to more complex structures,
like double [5] and layered perovskites [6] and new compounds of
interest for the light harvesting problem were found. In addition, the
trends in the bandgaps have been studied. The bandgaps can be tuned by
an opportune combination of the metal atoms in the B-ion position in
the double perovskite, and of the B-metal ion with the thickness of
the octahedra in the layered perovskite structure.
Thirdly, the possible crystal structures have been significantly
expanded by using the structures provided by the
Materials Project database, which is based on the experimental ICSD
database. The bandgaps were calculated again with the focus on finding
materials with potential as light harvesters. The results and the
possibilities for using the materials with different device designs
will be discussed.
References
[1] M. Kuisma, J. Ojanen, J. Enkovaara and T.T. Rantala, Physical
Review B 82, 115106 (2010).
[2] I.E. Castelli, T. Olsen, S. Datta, D.D. Landis, S. Dahl,
K.S. Thygesen and K.W. Jacobsen, Energy Environ. Sci. 5, 5814 (2012).
[3] I.E. Castelli, D.D. Landis, K.S. Thygesen, S. Dahl,
I. Chorkendorff, T.F. Jaramillo and K.W. Jacobsen, Energy
Environ. Sci. 5, 9034 (2012).
[4] I.E. Castelli, K.S. Thygesen, and K.W. Jacobsen, accepted Topics
in Catalysis (2013).
[5] I.E. Castelli, K.S. Thygesen, and K.W. Jacobsen, MRS Online
Proc. Libra. 1523 (2013).
[6] I.E. Castelli, J.M. Garcia-Lastra, F. Huser, K.S. Thygesen, and
K.W. Jacobsen, in printing New Journal of Physics (2013).
cell, where water is split into hydrogen and oxygen by solar light, is
one possible solution to the problem of increasing energy demand and
storage. A screening procedure based on ab-initio density
functional theory calculations has been applied to guide the search
for new materials. The main descriptors of the properties relevant for
the screening are: heat of formation, electronic bandgap, and
positions of the band edges with respect to the red-ox levels of
water. A recently implemented exchange-correlation functional, called
GLLB-SC [1], has been used for the estimation of the bandgaps.
Firstly, a screening procedure has been applied to 19000 cubic
perovskite structures. These are obtained by combining 52 metals
together with oxygen, nitrogen, sulfur and fluorine as anions. 32
promising materials have been found for visible light harvesting, 20
for the one-photon and 12 for the two-photon water splitting
process. In addition, 16 candidates were suggested for the
transparent shielding of the photocatalyst. The problem of corrosion
has been addressed for the candidates for the one-photon scheme using
Pourbaix diagrams [4].
Secondly, the screening has been extended to more complex structures,
like double [5] and layered perovskites [6] and new compounds of
interest for the light harvesting problem were found. In addition, the
trends in the bandgaps have been studied. The bandgaps can be tuned by
an opportune combination of the metal atoms in the B-ion position in
the double perovskite, and of the B-metal ion with the thickness of
the octahedra in the layered perovskite structure.
Thirdly, the possible crystal structures have been significantly
expanded by using the structures provided by the
Materials Project database, which is based on the experimental ICSD
database. The bandgaps were calculated again with the focus on finding
materials with potential as light harvesters. The results and the
possibilities for using the materials with different device designs
will be discussed.
References
[1] M. Kuisma, J. Ojanen, J. Enkovaara and T.T. Rantala, Physical
Review B 82, 115106 (2010).
[2] I.E. Castelli, T. Olsen, S. Datta, D.D. Landis, S. Dahl,
K.S. Thygesen and K.W. Jacobsen, Energy Environ. Sci. 5, 5814 (2012).
[3] I.E. Castelli, D.D. Landis, K.S. Thygesen, S. Dahl,
I. Chorkendorff, T.F. Jaramillo and K.W. Jacobsen, Energy
Environ. Sci. 5, 9034 (2012).
[4] I.E. Castelli, K.S. Thygesen, and K.W. Jacobsen, accepted Topics
in Catalysis (2013).
[5] I.E. Castelli, K.S. Thygesen, and K.W. Jacobsen, MRS Online
Proc. Libra. 1523 (2013).
[6] I.E. Castelli, J.M. Garcia-Lastra, F. Huser, K.S. Thygesen, and
K.W. Jacobsen, in printing New Journal of Physics (2013).