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Title: Electronic Structure, Phonon Dynamical Properties, and CO 2 Capture Capability of Na 2 - x M x Zr O 3 ( M = Li ,K): Density-Functional Calculations and Experimental Validations

Abstract

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. 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-dopedmore » 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

Authors:
 [1];  [1];  [2];  [2];  [3];  [3];  [4]
  1. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
  2. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States); West Virginia Univ., Morgantown, WV (United States). School of Medicine
  3. Univ. Nacional Autonoma de Mexico (UNAM), Mexico City (Mexico). Inst. de Investigaciones en Materiales
  4. Univ. of Minnesota, Minneapolis, MN (United States). School of Physics and Astronomy
Publication Date:
Research Org.:
National Energy Technology Lab. (NETL), Morgantown, WV (United States). In-house Research
Sponsoring Org.:
USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1178539
Report Number(s):
NETL-PUB-1163
Journal ID: ISSN 2331-7019; PRAHB2
Resource Type:
Journal Article
Journal Name:
Physical Review Applied
Additional Journal Information:
Journal Volume: 3; Journal Issue: 4; Journal ID: ISSN 2331-7019
Publisher:
American Physical Society
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 CO2 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 CO2 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 CO2 Capture Capability of Na2-xMxZrO3 ( M=Li ,K): Density-Functional Calculations and Experimental Validations". United States. doi:10.1103/PhysRevApplied.3.044013. https://www.osti.gov/servlets/purl/1178539.
@article{osti_1178539,
title = {Electronic Structure, Phonon Dynamical Properties, and CO2 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 = {The electronic structural and phonon properties of Na2-αMαZrO3 (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 CO2 absorption and desorption in these materials are also analyzed. With increasing doping level α, the binding energies of Na2-αLiαZrO3 are increased while the binding energies of Na2-α KαZrO3 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. 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 CO2 pressure, and the temperature of the CO2 capture reactions by Na2-αMαZrO3, and from thermogravimetric-analysis experimental measurements, the Li- and K-doped mixtures Na2-αMαZrO3 have lower turnover temperatures (Tt) and higher CO2 capture capacities, compared to pure Na2ZrO3. The Li-doped systems have a larger Tt decrease than the K-doped systems. When increasing the Li-doping level α, the Tt of the corresponding mixture Na2-αLiαZrO3 decreases further to a low-temperature range. However, in the case of K-doped systems Na2-αKαZrO3, although doping K into Na2ZrO3 initially shifts its Tt to lower temperatures, further increases of the K-doping level α causes Tt to increase. Therefore, doping Li into Na2ZrO3 has a larger influence on its CO2 capture performance than the K-doped Na2ZrO3. Compared with pure solidsM2ZrO3, after doping with other elements, these doped systems’ CO2 capture performances are improved.},
doi = {10.1103/PhysRevApplied.3.044013},
journal = {Physical Review Applied},
issn = {2331-7019},
number = 4,
volume = 3,
place = {United States},
year = {2015},
month = {4}
}