No data available.
Please log in to see this content.
You have no subscription access to this content.
No metrics data to plot.
The attempt to load metrics for this article has failed.
The attempt to plot a graph for these metrics has failed.
The full text of this article is not currently available.
orbital selective catalytic activity in brownmillerite Ca2
J. Suntivich, K. J. May, H. A. Gasteiger, J.B. Goodenough, and Y. Shao-Horn, “A perovskite oxide optimized for oxygen evolution catalysis from molecular orbital principles,” Science 334, 1383 (2011).
W. T. Hong et al., “Toward the rational design of non-precious transition metal oxides for oxygen electrocatalysis,” Energy Environ. Sci. 8, 1404 (2015).
J. Suntivich et al., “Design principles for oxygen-reduction activity on perovskite oxide catalysts for fuel cells and metal-air batteries,” Nat. Chem. 3, 546 (2011).
M. Risch et al., “La0.8Sr0.2MnO3-decorated with Ba0.5Sr0.5Co0.8Fe0.2O3-: a bifunctional surface for oxygen electrocatalysis with enhanced stability and activity,” J. Am. Chem. Soc. 136, 5229 (2014).
J. Kim, X. Yin, K. C. Tsao, S. Fang, and H. Yang, “Ca2Mn2O5 as oxygen-deficient perovskite electrocatalyst for oxygen evolution reaction,” J. Am. Chem. Soc. 136, 14646 (2014).
B. Hammer and J. K. Nørskov, “Theoretical surface science and catalysis—Calculations and concepts,” Adv. Catal. 45, 71 (2000).
A. Georges, G. Kotliar, W. Krauth, and M. J. Rozenberg, “Dynamical mean-field theory of strongly correlated fermion systems and the limit of infinite dimensions,” Reviews of Modern Physics 68, 13 (1996).
F. Lu, W.-H. Wang, and L.-J. Zou, “Metal-insulator transition in the half-filling two-orbital Hubbard model on the triangular lattice,” Physical Review B 77, 125117 (2008).
X. Deng, L. Wang, X. Dai, and Z. Fang, “Local density approximation combined with Gutzwiller method for correlated electron systems: Formalism and applications,” Physical Review B 79, 075114 (2009).
N. Marzari, A. A. Mostofi, J. R. Yates, I. Souza, and D. Vanderbilt, “Maximally localized Wannier functions: Theory and applications,” Reviews of Modern Physics 84, 1419 (2012).
D. Neagu, G. Tsekouras, D. N. Miller, H. Ménard, and J. T. Irvine, “In situ growth of nanoparticles through control of non-stoichiometry,” Nature Chemistry 5, 916–923 (2013).
Article metrics loading...
3d-orbital filling in transition metal oxide is crucial to govern the catalytic activity in oxygen evolution reduction, nevertheless, it is not fundamentally accessible why specific orbital occupation produces a highest catalytic performance. Here, we utilize brownmillerite Ca2Mn2O5 to clarify the orbital selective catalytic behavior due to the crystal field splitting and on-site coulomb interactions. Within density functional theory plus dynamical mean field theory, Ca2Mn2O5 shows a paramagnetic Mott insulating behavior at room temperature, consistent with optical adsorption spectra and magnetic susceptibility. As the center of the orbital locates in the lower Hubbard sub-band, the unit occupation on orbital provides a moderate bonding with external O* species to cause a high catalytic activity of Ca2Mn2O5 with a square pyramid crystal field. Such concept of unit occupation of near Fermi level could be extended to other crystal fields for future design of oxide catalysts.
Full text loading...
Most read this month