Antoine A. Emery
Current Organizations / Institutes
The organizations/institutes from the scholar's latest article
Research Subjects
Antoine A. Emery has a total of 23 co-authors. Here are the top co-authors by number of shared publications:
- Chris Wolverton
International Institute for Nanotechnology Northwestern University Evanston Illinois USA
4 shared publications Alex Zunger
Renewable and Sustainable Energy Institute, University of Colorado, Boulder, Colorado 80309, USA
1 shared publicationAnthony McDaniel
Sandia National Laboratory , Livermore , California , United States
1 shared publicationC. Bewerse
1 shared publicationChris Wolverton
Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA
1 shared publication- David Christophe Dunand
Department of Materials Science and Engineering, Northwestern University, Evanston, USA
1 shared publication
Latest Publications
- 30 May 2019
- Published by American Chemical Society (ACS) in Inorganic Chemistry
- Vol. 58 (12) , 7705-7714
Phase Identification of the Layered Perovskite CexSr2–xMnO4 and Application for Solar Thermochemical Water Splitting
Ruddlesden–Popper (layered perovskite) phases are attracting significant interest because of their unique potential for many applications requiring mixed ionic and electronic conductivity. Here we report a new, previously undiscovered layered perovskite of composition, CexSr2–xMnO4 (x = 0.1, 0.2, and 0.3). Furthermore, we demonstrate that this new system is suitable for solar thermochemical hydrogen production (STCH). Synchrotron radiation X-ray diffraction and transmission electron microscopy are performed to characterize this new system. Density functional theory calculations of phase stability and oxygen vacancy formation energy (1.76, 2.24, and 2.66 eV/O atom, respectively with increasing Ce content) reinforce the potential of this phase for STCH application. Experimental hydrogen production results show that this materials system produces 2–3 times more hydrogen than the benchmark STCH oxide ceria at a reduction temperature of 1400 °C and an oxidation temperature of 1000 °C.
- 30 May 2019
- Published by American Chemical Society (ACS) in Inorganic Chemistry
- Vol. 58 (12) , 7705-7714
Phase Identification of the Layered Perovskite CexSr2–xMnO4 and Application for Solar Thermochemical Water Splitting
Ruddlesden–Popper (layered perovskite) phases are attracting significant interest because of their unique potential for many applications requiring mixed ionic and electronic conductivity. Here we report a new, previously undiscovered layered perovskite of composition, CexSr2–xMnO4 (x = 0.1, 0.2, and 0.3). Furthermore, we demonstrate that this new system is suitable for solar thermochemical hydrogen production (STCH). Synchrotron radiation X-ray diffraction and transmission electron microscopy are performed to characterize this new system. Density functional theory calculations of phase stability and oxygen vacancy formation energy (1.76, 2.24, and 2.66 eV/O atom, respectively with increasing Ce content) reinforce the potential of this phase for STCH application. Experimental hydrogen production results show that this materials system produces 2–3 times more hydrogen than the benchmark STCH oxide ceria at a reduction temperature of 1400 °C and an oxidation temperature of 1000 °C.
- Open Access
- 11 April 2018
- Published by American Physical Society (APS) in Physical Review Materials
- Vol. 2 (4) , 043802
Predictions of new perovskite compounds by combining machine learning and density functional theoryWe apply machine learning (ML) methods to a database of 390 experimentally reported compounds to construct two statistical models that predict possible new perovskite materials and possible new cubic perovskites. The first ML model classified the 390 compounds into 254 perovskites and 136 that are not perovskites with a 90% average cross-validation (CV) accuracy; the second ML model further classified the perovskites into 22 known cubic perovskites and 232 known noncubic perovskites with a 94% average CV accuracy. We find that the most effective chemical descriptors affecting our classification include largely geometric constructs such as the and Shannon ionic radii, the tolerance and octahedral factors, the -O and -O bond length, and the and Villars' Mendeleev numbers. We then construct an additional list of compounds assembled from charge conserving combinations of and atoms absent from our list of known compounds. Then, using the two ML models constructed on the known compounds, we predict that 235 of the 625 exist in a perovskite structure with a confidence greater than 50% and among them that 20 exist in the cubic structure (albeit, the latter with only confidence). We find that the new perovskites are most likely to occur when the and atoms are a lanthanide or actinide, when the atom is an alkali, alkali earth, or late transition metal atom, or when the atom is a -block atom. We also compare the ML findings with the density functional theory calculations and convex hull analyses in the Open Quantum Materials Database (OQMD), which predicts the K ground-state stability of all the compounds. We find that OQMD predicts 186 of 254 of the perovskites in the experimental database to be thermodynamically stable within 100 meV/atom of the convex hull and predicts 87 of the 235 ML-predicted perovskite compounds to be thermodynamically stable within 100 meV/atom of the convex hull, including 6 of these to be in cubic structures. We suggest these 87 as the most promising candidates for future experimental synthesis of novel perovskites.- 11 April 2018
- Published by American Physical Society (APS) in Physical Review Materials
- Vol. 2 (4) , 043802
Open AccessPredictions of new perovskite compounds by combining machine learning and density functional theoryWe apply machine learning (ML) methods to a database of 390 experimentally reported compounds to construct two statistical models that predict possible new perovskite materials and possible new cubic perovskites. The first ML model classified the 390 compounds into 254 perovskites and 136 that are not perovskites with a 90% average cross-validation (CV) accuracy; the second ML model further classified the perovskites into 22 known cubic perovskites and 232 known noncubic perovskites with a 94% average CV accuracy. We find that the most effective chemical descriptors affecting our classification include largely geometric constructs such as the and Shannon ionic radii, the tolerance and octahedral factors, the -O and -O bond length, and the and Villars' Mendeleev numbers. We then construct an additional list of compounds assembled from charge conserving combinations of and atoms absent from our list of known compounds. Then, using the two ML models constructed on the known compounds, we predict that 235 of the 625 exist in a perovskite structure with a confidence greater than 50% and among them that 20 exist in the cubic structure (albeit, the latter with only confidence). We find that the new perovskites are most likely to occur when the and atoms are a lanthanide or actinide, when the atom is an alkali, alkali earth, or late transition metal atom, or when the atom is a -block atom. We also compare the ML findings with the density functional theory calculations and convex hull analyses in the Open Quantum Materials Database (OQMD), which predicts the K ground-state stability of all the compounds. We find that OQMD predicts 186 of 254 of the perovskites in the experimental database to be thermodynamically stable within 100 meV/atom of the convex hull and predicts 87 of the 235 ML-predicted perovskite compounds to be thermodynamically stable within 100 meV/atom of the convex hull, including 6 of these to be in cubic structures. We suggest these 87 as the most promising candidates for future experimental synthesis of novel perovskites. - Top Cited PapersOpen Access
- 17 October 2017
- Published by Springer Nature in Scientific Data
- Vol. 4 (1) , 170153
High-throughput DFT calculations of formation energy, stability and oxygen vacancy formation energy of ABO3 perovskites
ABO3 perovskites are oxide materials that are used for a variety of applications such as solid oxide fuel cells, piezo-, ferro-electricity and water splitting. Due to their remarkable stability with respect to cation substitution, new compounds for such applications potentially await discovery. In this work, we present an exhaustive dataset of formation energies of 5,329 cubic and distorted perovskites that were calculated using first-principles density functional theory. In addition to formation energies, several additional properties such as oxidation states, band gap, oxygen vacancy formation energy, and thermodynamic stability with respect to all phases in the Open Quantum Materials Database are also made publicly available. This large dataset for this ubiquitous crystal structure type contains 395 perovskites that are predicted to be thermodynamically stable, of which many have not yet been experimentally reported, and therefore represent theoretical predictions. The dataset thus opens avenues for future use, including materials discovery in many research-active areas.
- 17 October 2017
- Published by Springer Nature in Scientific Data
- Vol. 4 (1) , 170153
Top Cited PapersOpen AccessHigh-throughput DFT calculations of formation energy, stability and oxygen vacancy formation energy of ABO3 perovskites
ABO3 perovskites are oxide materials that are used for a variety of applications such as solid oxide fuel cells, piezo-, ferro-electricity and water splitting. Due to their remarkable stability with respect to cation substitution, new compounds for such applications potentially await discovery. In this work, we present an exhaustive dataset of formation energies of 5,329 cubic and distorted perovskites that were calculated using first-principles density functional theory. In addition to formation energies, several additional properties such as oxidation states, band gap, oxygen vacancy formation energy, and thermodynamic stability with respect to all phases in the Open Quantum Materials Database are also made publicly available. This large dataset for this ubiquitous crystal structure type contains 395 perovskites that are predicted to be thermodynamically stable, of which many have not yet been experimentally reported, and therefore represent theoretical predictions. The dataset thus opens avenues for future use, including materials discovery in many research-active areas.
- Open Access
- 18 August 2017
- Published by Springer Nature in Nature Communications
- Vol. 8 (1) , 1-6
Giant onsite electronic entropy enhances the performance of ceria for water splitting
Previous studies have shown that a large solid-state entropy of reduction increases the thermodynamic efficiency of metal oxides, such as ceria, for two-step thermochemical water splitting cycles. In this context, the configurational entropy arising from oxygen off-stoichiometry in the oxide, has been the focus of most previous work. Here we report a different source of entropy, the onsite electronic configurational entropy, arising from coupling between orbital and spin angular momenta in lanthanide f orbitals. We find that onsite electronic configurational entropy is sizable in all lanthanides, and reaches a maximum value of ≈4.7 kB per oxygen vacancy for Ce4+/Ce3+ reduction. This unique and large positive entropy source in ceria explains its excellent performance for high-temperature catalytic redox reactions such as water splitting. Our calculations also show that terbium dioxide has a high electronic entropy and thus could also be a potential candidate for solar thermochemical reactions.
- 18 August 2017
- Published by Springer Nature in Nature Communications
- Vol. 8 (1) , 1-6
Open AccessGiant onsite electronic entropy enhances the performance of ceria for water splitting
Previous studies have shown that a large solid-state entropy of reduction increases the thermodynamic efficiency of metal oxides, such as ceria, for two-step thermochemical water splitting cycles. In this context, the configurational entropy arising from oxygen off-stoichiometry in the oxide, has been the focus of most previous work. Here we report a different source of entropy, the onsite electronic configurational entropy, arising from coupling between orbital and spin angular momenta in lanthanide f orbitals. We find that onsite electronic configurational entropy is sizable in all lanthanides, and reaches a maximum value of ≈4.7 kB per oxygen vacancy for Ce4+/Ce3+ reduction. This unique and large positive entropy source in ceria explains its excellent performance for high-temperature catalytic redox reactions such as water splitting. Our calculations also show that terbium dioxide has a high electronic entropy and thus could also be a potential candidate for solar thermochemical reactions.
- Top Cited Papers
- 7 July 2016
- Published by American Chemical Society (ACS) in Chemistry of Materials
- Vol. 28 (16) , 5621-5634
High-Throughput Computational Screening of Perovskites for Thermochemical Water Splitting Applications
- 7 July 2016
- Published by American Chemical Society (ACS) in Chemistry of Materials
- Vol. 28 (16) , 5621-5634
Top Cited PapersHigh-Throughput Computational Screening of Perovskites for Thermochemical Water Splitting Applications
- 1 May 2015
- Published by Elsevier in Materials Science and Engineering: A
- Vol. 634, 153-160
NiTi porous structure with 3D interconnected microchannels using steel wire spaceholders
- 1 May 2015
- Published by Elsevier in Materials Science and Engineering: A
- Vol. 634, 153-160
NiTi porous structure with 3D interconnected microchannels using steel wire spaceholders