Prediction of solid oxide fuel cell cathode activity with first-principles descriptors

Lee, Yueh‐Lin; Kleis, Jesper; Rossmeisl, Jan; Shao‐Horn, Yang; Morgan, Dane

doi:10.1039/c1ee02032c

Cited by 533 publications

(620 citation statements)

References 62 publications

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“…This weakening is consistent with the work of Garcia-Mota et al 22 and was also revealed in our previous work 34 , where surface adsorption energies upon inclusion of Hubbard U correction has been shown to correlate with shift downward of O 2p-band center relative to the Fermi level ( Figure S2 of Ref. 58 ). An further weakening effect for hybrid functionals was shown by Wang et al 15 for ΔE(HO*), ΔE(O*), and ΔE(HOO*) adsorption energies by comparing the hybrid functional results to those calculated with the GGA+U approach.…”

Section: Surface Adsorption Energies and The Scaling Relationship Forsupporting

confidence: 92%

“…We first made a direct comparison of results calculated at the GGA+U level with the results calculated at the GGA level 14 , for assessment of the effect of including Hubbard U corrections on the surface adsorption energies and their scaling relationship, as well as the predicted ORR/OER activities. In addition, we examined the trends between the adsorption energies and the electronic structure descriptors, i.e., d-electron filling of the transition metals 1,8 as well as the O 2p-band center relative the Fermi level 58 . We revealed that an excellent correlation exists between the sub-surface layer O 2p-band center and the computed (001) AO and BO 2 bare surface HO* adsorption energies, which can be attributed to shifts of surface electron energy level near the surfaces due to compensating surface charge from bulk polarity (i.e.…”

Section: Results-predicted Orr and Oer Activitiesmentioning

confidence: 99%

“…In the following discussions, we examined the trends of surface HO* adsorption energies vs. selected first principles based electronic structure descriptors, including d-electron filling of the transition metals 1,8 as well as the O 2p-band center relative the Fermi level 58 .…”

Section: Surface Ho* Adsorption Energies Vs Electronic Structure Desmentioning

confidence: 99%

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Ab initio GGA+U study of oxygen evolution and oxygen reduction electrocatalysis on the (001) surfaces of lanthanum transition metal perovskites LaBO₃(B = Cr, Mn, Fe, Co and Ni)

Lee

Gadre

Shao‐Horn

et al. 2015

Phys. Chem. Chem. Phys.

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109

135

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ARTICLEThis journal is © The Royal Society of Chemistry 2013 J. Name., 2013, 00, 1--3 | 1 A IntroductionSearch and design of highly active and less expensive materials for catalyzing the sluggish kinetics of the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is of primary importance in many electrochemical energy device applications such as direct-solar and electrolytic water splitting, metal-air batteries, and fuel cells [1][2][3][4][5][6] . In replacement of noble metal containing catalysts, first row transition-metal perovskites are promising candidate materials for catalyzing OER and ORR in alkaline solution. A number of activity descriptor approaches provide an efficient and practical guidance to facilitate screening of alternate perovskite OER and ORR catalysts 4,5,7 , such as number of d-electrons 1, 8 , oxidation enthalpy 1, 9 , the p-band center relative to the Fermi level 6 , the degree of overlapping between the e g orbitals of the M(3d) band and the O(2p) band relative to the Fermi level 10 , and free energies of formation of the bulk perovskites relative to metal and H 2 O/H 2 11. However, there are still many questions about surfaces and interfaces of the transition-metal perovskite catalyst systems in the aqueous environment under the OER and ORR conditions which have invoked further experimental studies 12,13 . These questions include, e.g., what are the stable surfaces for these perovskites, how different surface orientations/terminations result in different activities, how the bulk electronic structure descriptors can be used to describe activities of various surface terminations, and whether/how surface stability is linked to surface catalytic activities. First principles-based Density Functional Theory (DFT) methods are now able to simulate catalytic reactions at specific metal oxide surfaces and extract surface electronic structure and energetic details, which can provide new insights into structure-activity relationships and strategies for material design and development 7,[14][15][16] . For example, Man et al. 14 have performed

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Section: Surface Adsorption Energies and The Scaling Relationship Forsupporting

confidence: 92%

Section: Results-predicted Orr and Oer Activitiesmentioning

confidence: 99%

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Ab initio GGA+U study of oxygen evolution and oxygen reduction electrocatalysis on the (001) surfaces of lanthanum transition metal perovskites LaBO₃(B = Cr, Mn, Fe, Co and Ni)

Lee

Gadre

Shao‐Horn

et al. 2015

Phys. Chem. Chem. Phys.

Self Cite

109

135

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“…Recent experimental and computational work has indicated that the d-band model is not applicable to oxides [160]. Other descriptors, such as e g -state occupancy, the covalency of the transition metal-oxygen bond for low-temperature ORR activity in water, the O 2p band center energy, and the minority electronic carrier density in the conduction band of the material have been proposed [160][161][162]. However, none of these seem to work for oxides in general.…”

Section: Strain Segregation and Reactivitymentioning

confidence: 99%

“…Electronic structure also plays a major role in influencing surface oxygen reduction reactivity, as has been illustrated by examples in several oxides [55,[160][161][162]. Using in situ STM/S, Yildiz et al conducted a series of studies on the surface electronic structure of tensile and compressive-strained (La,Sr)CoO 3 and (La,Sr)MnO 3 at high temperature in an oxygen environment [45,53].…”

Section: Strain Segregation and Reactivitymentioning

confidence: 99%

Chemomechanics of ionically conductive ceramics for electrical energy conversion and storage

et al. 2014

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Functional materials for energy conversion and storage exhibit strong coupling between electrochemistry and mechanics. For example, ceramics developed as electrodes for both solid oxide fuel cells and batteries exhibit cyclic volumetric expansion upon reversible ion transport. Such chemomechanical coupling is typically far from thermodynamic equilibrium, and thus is challenging to quantify experimentally and computationally. In situ measurements and atomistic simulations are under rapid development to explore how this coupling can be used to potentially improve both device performance and durability. Here, we review the commonalities of coupling between electrochemical and mechanical states in fuel cell and battery materials, illustrating with specific cases the progress in materials processing, in situ characterization, and computational modeling and simulation. We also highlight outstanding questions and opportunities in these applications -both to better understand the limiting mechanisms within the materials and to significantly advance the durability and predictability of device performance required for renewable energy conversion and storage.

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Energy Conversion: Solid Oxide Fuel Cells: First‐Principles Modeling of Elementary Processes

Kotomin¹,

Merkle²,

Mastrikov³

et al. 2013

Computational Approaches to Energy Materials

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Prediction of solid oxide fuel cell cathode activity with first-principles descriptors

Cited by 533 publications

References 62 publications

Ab initio GGA+U study of oxygen evolution and oxygen reduction electrocatalysis on the (001) surfaces of lanthanum transition metal perovskites LaBO₃(B = Cr, Mn, Fe, Co and Ni)

Ab initio GGA+U study of oxygen evolution and oxygen reduction electrocatalysis on the (001) surfaces of lanthanum transition metal perovskites LaBO₃(B = Cr, Mn, Fe, Co and Ni)

Chemomechanics of ionically conductive ceramics for electrical energy conversion and storage

Energy Conversion: Solid Oxide Fuel Cells: First‐Principles Modeling of Elementary Processes

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Prediction of solid oxide fuel cell cathode activity with first-principles descriptors

Cited by 533 publications

References 62 publications

Ab initio GGA+U study of oxygen evolution and oxygen reduction electrocatalysis on the (001) surfaces of lanthanum transition metal perovskites LaBO3(B = Cr, Mn, Fe, Co and Ni)

Ab initio GGA+U study of oxygen evolution and oxygen reduction electrocatalysis on the (001) surfaces of lanthanum transition metal perovskites LaBO3(B = Cr, Mn, Fe, Co and Ni)

Chemomechanics of ionically conductive ceramics for electrical energy conversion and storage

Energy Conversion: Solid Oxide Fuel Cells: First‐Principles Modeling of Elementary Processes

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Product

Resources

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Ab initio GGA+U study of oxygen evolution and oxygen reduction electrocatalysis on the (001) surfaces of lanthanum transition metal perovskites LaBO₃(B = Cr, Mn, Fe, Co and Ni)

Ab initio GGA+U study of oxygen evolution and oxygen reduction electrocatalysis on the (001) surfaces of lanthanum transition metal perovskites LaBO₃(B = Cr, Mn, Fe, Co and Ni)