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Title: Electronic Structure, Phonon Dynamical Properties, and Capture Capability of Na2-xMxZrO3 (M=Li,K): Density-Functional Calculations and Experimental Validations

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
National Energy Technology Lab. (NETL), Pittsburgh, PA, and Morgantown, WV (United States). In-house Research
Sponsoring Org.:
USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1225777
Report Number(s):
A-NETL-PUB-118
Journal ID: ISSN 2331-7019: PRAHB2
Resource Type:
Journal Article
Resource Relation:
Journal Name: Physical Review Applied; Journal Volume: 3; Journal Issue: 4
Country of Publication:
United States
Language:
English

Citation Formats

Duan, Yuhua, Lekse, Jonathan, Wang, Xianfeng, Li, Bingyun, Alcántar-Vázquez, Brenda, Pfeiffer, Heriberto, and Halley, J. W. Electronic Structure, Phonon Dynamical Properties, and Capture Capability of Na2-xMxZrO3 (M=Li,K): Density-Functional Calculations and Experimental Validations. United States: N. p., 2015. Web. doi:10.1103/PhysRevApplied.3.044013.
Duan, Yuhua, Lekse, Jonathan, Wang, Xianfeng, Li, Bingyun, Alcántar-Vázquez, Brenda, Pfeiffer, Heriberto, & Halley, J. W. Electronic Structure, Phonon Dynamical Properties, and Capture Capability of Na2-xMxZrO3 (M=Li,K): Density-Functional Calculations and Experimental Validations. United States. doi:10.1103/PhysRevApplied.3.044013.
Duan, Yuhua, Lekse, Jonathan, Wang, Xianfeng, Li, Bingyun, Alcántar-Vázquez, Brenda, Pfeiffer, Heriberto, and Halley, J. W. Wed . "Electronic Structure, Phonon Dynamical Properties, and Capture Capability of Na2-xMxZrO3 (M=Li,K): Density-Functional Calculations and Experimental Validations". United States. doi:10.1103/PhysRevApplied.3.044013.
@article{osti_1225777,
title = {Electronic Structure, Phonon Dynamical Properties, and Capture Capability of Na2-xMxZrO3 (M=Li,K): Density-Functional Calculations and Experimental Validations},
author = {Duan, Yuhua and Lekse, Jonathan and Wang, Xianfeng and Li, Bingyun and Alcántar-Vázquez, Brenda and Pfeiffer, Heriberto and Halley, J. W.},
abstractNote = {},
doi = {10.1103/PhysRevApplied.3.044013},
journal = {Physical Review Applied},
number = 4,
volume = 3,
place = {United States},
year = {Wed Apr 01 00:00:00 EDT 2015},
month = {Wed Apr 01 00:00:00 EDT 2015}
}
  • The electronic structural and phonon properties of Na 2-αM αZrO 3 (M ¼ Li,K, α = ¼ 0.0,0.5,1.0,1.5,2.0) are investigated by first-principles density-functional theory and phonon dynamics. The thermodynamic properties of CO 2 absorption and desorption in these materials are also analyzed. With increasing doping level α, the binding energies of Na 2-αLi αZrO 3 are increased while the binding energies of Na 2-α K αZrO 3 are decreased to destabilize the structures. The calculated band structures and density of states also show that, at the same doping level, the doping sites play a significant role in the electronic properties.more » The phonon dispersion results show that few soft modes are found in several doped configurations, which indicates that these structures are less stable than other configurations with different doping levels. From the calculated relationships among the chemical-potential change, the CO 2 pressure, and the temperature of the CO 2 capture reactions by Na 2-αM αZrO 3, and from thermogravimetric-analysis experimental measurements, the Li- and K-doped mixtures Na 2-αM αZrO 3 have lower turnover temperatures (T t) and higher CO 2 capture capacities, compared to pure Na 2ZrO 3. The Li-doped systems have a larger T t decrease than the K-doped systems. When increasing the Li-doping level α, the T t of the corresponding mixture Na 2-αLi αZrO 3 decreases further to a low-temperature range. However, in the case of K-doped systems Na 2-αK αZrO 3, although doping K into Na 2ZrO 3 initially shifts its T t to lower temperatures, further increases of the K-doping level α causes T t to increase. Therefore, doping Li into Na 2ZrO 3 has a larger influence on its CO 2 capture performance than the K-doped Na 2ZrO 3. Compared with pure solidsM 2ZrO 3, after doping with other elements, these doped systems’ CO 2 capture performances are improved.« less
  • We have computed the phase diagrams for multi-component M-C-O-H (M=Li, Na, K) systems using firstprinciples density functional theory complemented with lattice phonon calculations. We have identified all CO 2 capture reactions that lie on the Gibbs free energy convex hull as a function of temperature and the partial pressures of CO 2 and H 2O. Our predicted phase diagrams for CO 2 capture reactions are in qualitative and in some instances quantitative agreement with experimental data. The Na 2CO 3/NaHCO 3 and K 2CO 3/KHCO 3 systems were found to be the most promising candidates of all those we investigatedmore » for both pre- and post-combustion CO 2 capture. Overall, we show that our calculation approach can be used to screen promising materials for CO 2 capture under different conditions of temperature and pressure.« less
  • We have computed the phase diagrams for multi-component M–C–O–H (M=Li, Na, K) systems using first-principles density functional theory complemented with lattice phonon calculations. We have identified all CO{sub 2} capture reactions that lie on the Gibbs free energy convex hull as a function of temperature and the partial pressures of CO{sub 2} and H{sub 2}O. Our predicted phase diagrams for CO{sub 2} capture reactions are in qualitative and in some instances quantitative agreement with experimental data. The Na{sub 2}CO{sub 3}/NaHCO{sub 3} and K{sub 2}CO{sub 3}/KHCO{sub 3} systems were found to be the most promising candidates of all those we investigatedmore » for both pre- and post-combustion CO{sub 2} capture. Overall, we show that our calculation approach can be used to screen promising materials for CO{sub 2} capture under different conditions of temperature and pressure.« less
  • We have computed the phase diagrams for multi-component M-C-O-H (M=Li, Na, K) systems using first-principles density functional theory complemented with lattice phonon calculations. We have identified all CO{sub 2} capture reactions that lie on the Gibbs free energy convex hull as a function of temperature and the partial pressures of CO{sub 2} and H{sub 2}O. Our predicted phase diagrams for CO{sub 2} capture reactions are in qualitative and in some instances quantitative agreement with experimental data. The Na{sub 2}CO{sub 3}/NaHCO{sub 3} and K{sub 2}CO{sub 3}/KHCO{sub 3} systems were found to be the most promising candidates of all those we investigatedmore » for both pre- and post-combustion CO{sub 2} capture. Overall, we show that our calculation approach can be used to screen promising materials for CO{sub 2} capture under different conditions of temperature and pressure. -- Graphical abstract: The calculated results indicate that the Na{sub 2}CO{sub 3}/NaHCO{sub 3} and K{sub 2}CO{sub 3}/KHCO{sub 3} systems are the most promising candidates of all those we investigated for both pre-and post-combustion CO{sub 2} capture. Display Omitted Research highlights: > Calculated the phase diagrams for multi-component M-C-O-H (M=Li, Na, K) systems. > Identified all CO{sub 2} capture reactions that lie on the Gibbs free energy convex hull. > Predicted phase diagrams for CO{sub 2} capture reactions are close to experimental data. > The Na{sub 2}CO{sub 3}/NaHCO{sub 3} and K{sub 2}CO{sub 3}/KHCO{sub 3} systems are the most promising candidates. > Our approach can be used to screen promising materials for CO{sub 2} capture.« less