Assessing Correlations of Perovskite Catalytic Performance with Electronic Structure Descriptors
Abstract
Electronic structure descriptors are computationally efficient quantities used to construct qualitative correlations for a variety of properties. In particular, the oxygen p-band center has been used to guide material discovery and fundamental understanding of an array of perovskite compounds for use in catalyzing the oxygen reduction and evolution reactions. Yet, an assessment of the effectiveness of the oxygen p-band center at predicting key measures of perovskite catalytic activity has not been made and would be highly beneficial to guide future predictions and codify best practices. In this work, we have used density functional theory at the Perdew–Burke–Ernzerhof (PBE), PBEsol, PBE + U, strongly constrained and appropriately normed functional, and Heyd–Scuseria–Ernzerhof (HSE06) levels to assess the correlations of numerous measures of catalytic performance for a series of technologically relevant perovskite oxides, using the bulk oxygen p-band center as an electronic structure descriptor. We have analyzed correlations of the calculated oxygen p-band center for all considered functionals with the experimentally measured X-ray emission spectroscopy oxygen p-band center and multiple measures of catalytic activity, including high-temperature oxygen reduction surface exchange rates, aqueous oxygen evolution current densities, and binding energies of oxygen evolution intermediate species. Our findings show that the best correlations for allmore »
- Authors:
-
- Univ. of Wisconsin−Madison, Madison, WI (United States)
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- Sponsoring Org.:
- USDOE; University of Wisconsin–Madison Center For High Throughput Computing (CHTC)
- OSTI Identifier:
- 1543616
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 31; Journal Issue: 3; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Jacobs, Ryan, Hwang, Jonathan, Shao-Horn, Yang, and Morgan, Dane. Assessing Correlations of Perovskite Catalytic Performance with Electronic Structure Descriptors. United States: N. p., 2019.
Web. doi:10.1021/acs.chemmater.8b03840.
Jacobs, Ryan, Hwang, Jonathan, Shao-Horn, Yang, & Morgan, Dane. Assessing Correlations of Perovskite Catalytic Performance with Electronic Structure Descriptors. United States. https://doi.org/10.1021/acs.chemmater.8b03840
Jacobs, Ryan, Hwang, Jonathan, Shao-Horn, Yang, and Morgan, Dane. Fri .
"Assessing Correlations of Perovskite Catalytic Performance with Electronic Structure Descriptors". United States. https://doi.org/10.1021/acs.chemmater.8b03840. https://www.osti.gov/servlets/purl/1543616.
@article{osti_1543616,
title = {Assessing Correlations of Perovskite Catalytic Performance with Electronic Structure Descriptors},
author = {Jacobs, Ryan and Hwang, Jonathan and Shao-Horn, Yang and Morgan, Dane},
abstractNote = {Electronic structure descriptors are computationally efficient quantities used to construct qualitative correlations for a variety of properties. In particular, the oxygen p-band center has been used to guide material discovery and fundamental understanding of an array of perovskite compounds for use in catalyzing the oxygen reduction and evolution reactions. Yet, an assessment of the effectiveness of the oxygen p-band center at predicting key measures of perovskite catalytic activity has not been made and would be highly beneficial to guide future predictions and codify best practices. In this work, we have used density functional theory at the Perdew–Burke–Ernzerhof (PBE), PBEsol, PBE + U, strongly constrained and appropriately normed functional, and Heyd–Scuseria–Ernzerhof (HSE06) levels to assess the correlations of numerous measures of catalytic performance for a series of technologically relevant perovskite oxides, using the bulk oxygen p-band center as an electronic structure descriptor. We have analyzed correlations of the calculated oxygen p-band center for all considered functionals with the experimentally measured X-ray emission spectroscopy oxygen p-band center and multiple measures of catalytic activity, including high-temperature oxygen reduction surface exchange rates, aqueous oxygen evolution current densities, and binding energies of oxygen evolution intermediate species. Our findings show that the best correlations for all measures of catalytic activity considered here are made with PBE-level calculations, with strong observed linear correlations with the bulk oxygen p-band center (R2 = 0.81–0.87). This study illustrates that strong linear correlations between numerous important measures of catalytic activity and the oxygen p-band bulk descriptor can be obtained under a consistent computational framework, and these correlations can serve as a guide for future experiments and simulations for development of perovskite and related oxide catalysts.},
doi = {10.1021/acs.chemmater.8b03840},
journal = {Chemistry of Materials},
number = 3,
volume = 31,
place = {United States},
year = {Fri Jan 04 00:00:00 EST 2019},
month = {Fri Jan 04 00:00:00 EST 2019}
}
Web of Science
Works referenced in this record:
Efficient hybrid density functional calculations in solids: Assessment of the Heyd–Scuseria–Ernzerhof screened Coulomb hybrid functional
journal, July 2004
- Heyd, Jochen; Scuseria, Gustavo E.
- The Journal of Chemical Physics, Vol. 121, Issue 3, p. 1187-1192
Surface strontium enrichment on highly active perovskites for oxygen electrocatalysis in solid oxide fuel cells
journal, January 2012
- Crumlin, Ethan J.; Mutoro, Eva; Liu, Zhi
- Energy & Environmental Science, Vol. 5, Issue 3
Computational high-throughput screening of electrocatalytic materials for hydrogen evolution
journal, October 2006
- Greeley, Jeff; Jaramillo, Thomas F.; Bonde, Jacob
- Nature Materials, Vol. 5, Issue 11, p. 909-913
Fuel cell materials and components☆☆☆The Golden Jubilee Issue—Selected topics in Materials Science and Engineering: Past, Present and Future, edited by S. Suresh.
journal, November 2003
- Haile, Sossina M.
- Acta Materialia, Vol. 51, Issue 19
Changing the Activity of Electrocatalysts for Oxygen Reduction by Tuning the Surface Electronic Structure
journal, April 2006
- Stamenkovic, Vojislav; Mun, Bongjin Simon; Mayrhofer, Karl J. J.
- Angewandte Chemie International Edition, Vol. 45, Issue 18
Hybrid functionals based on a screened Coulomb potential
journal, May 2003
- Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
- The Journal of Chemical Physics, Vol. 118, Issue 18
Estimating Hybridization of Transition Metal and Oxygen States in Perovskites from O K -edge X-ray Absorption Spectroscopy
journal, January 2014
- Suntivich, Jin; Hong, Wesley T.; Lee, Yueh-Lin
- The Journal of Physical Chemistry C, Vol. 118, Issue 4
Electronic factors determining the reactivity of metal surfaces
journal, December 1995
- Hammer, B.; Nørskov, J. K.
- Surface Science, Vol. 343, Issue 3
Oxygen tracer diffusion and surface exchange kinetics in La0.6Sr0.4CoO3−δ
journal, June 2010
- Berenov, A. V.; Atkinson, A.; Kilner, J. A.
- Solid State Ionics, Vol. 181, Issue 17-18
Oxygen Point Defect Chemistry in Ruddlesden–Popper Oxides (La 1– x Sr x ) 2 MO 4±δ (M = Co, Ni, Cu)
journal, May 2016
- Xie, Wei; Lee, Yueh-Lin; Shao-Horn, Yang
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 10
Energy band gaps and lattice parameters evaluated with the Heyd-Scuseria-Ernzerhof screened hybrid functional
journal, November 2005
- Heyd, Jochen; Peralta, Juan E.; Scuseria, Gustavo E.
- The Journal of Chemical Physics, Vol. 123, Issue 17
The Electrocatalysis of Oxygen Evolution on Perovskites
journal, January 1984
- Bockris, John O'M.
- Journal of The Electrochemical Society, Vol. 131, Issue 2
Double perovskites as a family of highly active catalysts for oxygen evolution in alkaline solution
journal, September 2013
- Grimaud, Alexis; May, Kevin J.; Carlton, Christopher E.
- Nature Communications, Vol. 4, Issue 1
Voltage, stability and diffusion barrier differences between sodium-ion and lithium-ion intercalation materials
journal, January 2011
- Ong, Shyue Ping; Chevrier, Vincent L.; Hautier, Geoffroy
- Energy & Environmental Science, Vol. 4, Issue 9
First principles computational materials design for energy storage materials in lithium ion batteries
journal, January 2009
- Meng, Ying Shirley; Arroyo-de Dompablo, M. Elena
- Energy & Environmental Science, Vol. 2, Issue 6
Accurate Band Gaps for Semiconductors from Density Functional Theory
journal, January 2011
- Xiao, Hai; Tahir-Kheli, Jamil; Goddard, William A.
- The Journal of Physical Chemistry Letters, Vol. 2, Issue 3
First-principles calculations of the electronic structure and spectra of strongly correlated systems: the LDA + U method
journal, January 1997
- Anisimov, Vladimir I.; Aryasetiawan, F.; Lichtenstein, A. I.
- Journal of Physics: Condensed Matter, Vol. 9, Issue 4, p. 767-808
Why Is Bulk Thermochemistry a Good Descriptor for the Electrocatalytic Activity of Transition Metal Oxides?
journal, January 2015
- Calle-Vallejo, Federico; Díaz-Morales, Oscar A.; Kolb, Manuel J.
- ACS Catalysis, Vol. 5, Issue 2
Scaling Relationships for Adsorption Energies on Transition Metal Oxide, Sulfide, and Nitride Surfaces
journal, June 2008
- Fernández, Eva M.; Moses, Poul G.; Toftelund, Anja
- Angewandte Chemie International Edition, Vol. 47, Issue 25
Material Discovery and Design Principles for Stable, High Activity Perovskite Cathodes for Solid Oxide Fuel Cells
journal, January 2018
- Jacobs, Ryan; Mayeshiba, Tam; Booske, John
- Advanced Energy Materials, Vol. 8, Issue 11
Factors controlling oxygen migration barriers in perovskites
journal, November 2016
- Mayeshiba, Tam T.; Morgan, Dane D.
- Solid State Ionics, Vol. 296
Accurate first-principles structures and energies of diversely bonded systems from an efficient density functional
journal, June 2016
- Sun, Jianwei; Remsing, Richard C.; Zhang, Yubo
- Nature Chemistry, Vol. 8, Issue 9
Hybrid functionals applied to perovskites
journal, May 2014
- Franchini, Cesare
- Journal of Physics: Condensed Matter, Vol. 26, Issue 25
A Perovskite Oxide Optimized for Oxygen Evolution Catalysis from Molecular Orbital Principles
journal, October 2011
- Suntivich, J.; May, K. J.; Gasteiger, H. A.
- Science, Vol. 334, Issue 6061
Understanding and Controlling the Work Function of Perovskite Oxides Using Density Functional Theory
journal, May 2016
- Jacobs, Ryan; Booske, John; Morgan, Dane
- Advanced Functional Materials, Vol. 26, Issue 30
The Li intercalation potential of LiMPO4 and LiMSiO4 olivines with M=Fe, Mn, Co, Ni
journal, November 2004
- Zhou, Fei; Cococcioni, Matteo; Kang, Kisuk
- Electrochemistry Communications, Vol. 6, Issue 11, p. 1144-1148
Activating lattice oxygen redox reactions in metal oxides to catalyse oxygen evolution
journal, January 2017
- Grimaud, Alexis; Diaz-Morales, Oscar; Han, Binghong
- Nature Chemistry, Vol. 9, Issue 5
Kinetics of Oxygen Surface Exchange on Epitaxial Ruddlesden–Popper Phases and Correlations to First-Principles Descriptors
journal, January 2016
- Lee, Yueh-Lin; Lee, Dongkyu; Wang, Xiao Renshaw
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 2
Stretching Epitaxial La 0.6 Sr 0.4 CoO 3−δ for Fast Oxygen Reduction
journal, November 2017
- Lee, Dongkyu; Jacobs, Ryan; Jee, Youngseok
- The Journal of Physical Chemistry C, Vol. 121, Issue 46
Accurate treatment of solids with the HSE screened hybrid
journal, October 2010
- Henderson, Thomas M.; Paier, Joachim; Scuseria, Gustavo E.
- physica status solidi (b), Vol. 248, Issue 4
Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces
journal, March 2011
- Man, Isabela C.; Su, Hai‐Yan; Calle‐Vallejo, Federico
- ChemCatChem, Vol. 3, Issue 7
Why gold is the noblest of all the metals
journal, July 1995
- Hammer, B.; Norskov, J. K.
- Nature, Vol. 376, Issue 6537
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation
journal, July 2013
- Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy
- APL Materials, Vol. 1, Issue 1
A high-performance cathode for the next generation of solid-oxide fuel cells
journal, September 2004
- Shao, Zongping; Haile, Sossina M.
- Nature, Vol. 431, Issue 7005, p. 170-173
Oxygen Reduction Activity on Perovskite Oxide Surfaces: A Comparative First-Principles Study of LaMnO 3 , LaFeO 3 , and LaCrO 3
journal, January 2013
- Wang, Yan; Cheng, Hai-Ping
- The Journal of Physical Chemistry C, Vol. 117, Issue 5
Materials for Solid Oxide Fuel Cells †
journal, February 2010
- Jacobson, Allan J.
- Chemistry of Materials, Vol. 22, Issue 3
Prediction of solid oxide fuel cell cathode activity with first-principles descriptors
journal, January 2011
- Lee, Yueh-Lin; Kleis, Jesper; Rossmeisl, Jan
- Energy & Environmental Science, Vol. 4, Issue 10
Probing LaMO 3 Metal and Oxygen Partial Density of States Using X-ray Emission, Absorption, and Photoelectron Spectroscopy
journal, January 2015
- Hong, Wesley T.; Stoerzinger, Kelsey A.; Moritz, Brian
- The Journal of Physical Chemistry C, Vol. 119, Issue 4
Modification of the surface electronic and chemical properties of Pt(111) by subsurface 3d transition metals
journal, June 2004
- Kitchin, J. R.; Nørskov, J. K.; Barteau, M. A.
- The Journal of Chemical Physics, Vol. 120, Issue 21
Toward the rational design of non-precious transition metal oxides for oxygen electrocatalysis
journal, January 2015
- Hong, Wesley T.; Risch, Marcel; Stoerzinger, Kelsey A.
- Energy & Environmental Science, Vol. 8, Issue 5
Electron correlations in narrow energy bands
journal, November 1963
- Hubbard, J.
- Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences, Vol. 276, Issue 1365, p. 238-257
Number of outer electrons as descriptor for adsorption processes on transition metals and their oxides
journal, January 2013
- Calle-Vallejo, Federico; Inoglu, Nilay G.; Su, Hai-Yan
- Chemical Science, Vol. 4, Issue 3
Towards the computational design of solid catalysts
journal, April 2009
- Nørskov, J.; Bligaard, T.; Rossmeisl, J.
- Nature Chemistry, Vol. 1, Issue 1, p. 37-46
Design principles for oxygen-reduction activity on perovskite oxide catalysts for fuel cells and metal–air batteries
journal, June 2011
- Suntivich, Jin; Gasteiger, Hubert A.; Yabuuchi, Naoaki
- Nature Chemistry, Vol. 3, Issue 7, p. 546-550
Screened Hybrid Exact Exchange Correction Scheme for Adsorption Energies on Perovskite Oxides
journal, July 2015
- Santos, Elton J. G.; Nørskov, Jens K.; Vojvodic, A.
- The Journal of Physical Chemistry C, Vol. 119, Issue 31
Alloys of platinum and early transition metals as oxygen reduction electrocatalysts
journal, September 2009
- Greeley, J.; Stephens, I. E. L.; Bondarenko, A. S.
- Nature Chemistry, Vol. 1, Issue 7, p. 552-556
High-throughput computational screening for low work function perovskite electron emitters
conference, April 2017
- Jacobs, Ryan; Morgan, Dane; Booske, John
- 2017 Eighteenth International Vacuum Electronics Conference (IVEC)
Works referencing / citing this record:
Quadruple perovskite ruthenate as a highly efficient catalyst for acidic water oxidation
journal, August 2019
- Miao, Xianbing; Zhang, Lifu; Wu, Liang
- Nature Communications, Vol. 10, Issue 1
Activity‐Stability Volcano Plots for Material Optimization in Electrocatalysis
journal, June 2019
- Exner, Kai S.
- ChemCatChem, Vol. 11, Issue 14
Two-dimensional ZnO for the selective photoreduction of CO 2
journal, January 2019
- Zhao, Yanyan; Liu, Nanshu; Zhou, Si
- Journal of Materials Chemistry A, Vol. 7, Issue 27
Quadruple perovskite ruthenate as a highly efficient catalyst for acidic water oxidation
journal, August 2019
- Miao, Xianbing; Zhang, Lifu; Wu, Liang
- Nature Communications, Vol. 10, Issue 1