The carrier concentration, the lattice constant, oxygen vacancies, mobility, and estimated
Abstract
Oxide thermoelectric materials are considered promising for high-temperature thermoelectric applications in terms of low cost, temperature stability, reversible reaction, and so on. Oxide materials have been intensively studied to suppress the defects and electronic charge carriers for many electronic device applications, but the studies with a high concentration of defects are limited. It desires to improve thermoelectric performance by enhancing its charge transport and lowering its lattice thermal conductivity. For this purpose, here, we modified the stoichiometry of cation and anion vacancies in two different systems to regulate the carrier concentration and explored their thermoelectric properties. Both cation and anion vacancies act as a donor of charge carriers and act as phonon scattering centers, decoupling the electrical conductivity and thermal conductivity.
Keywords
- thermoelectrics
- nonstoichiometry
- defect
- phonon scattering
- conductive oxide
- charge transport
1. Introduction
The demand for alternate energy of fossil fuel becomes a challenging task for the researcher and scientist. A possible strategy for an alternate energy source is thermoelectric (TE) materials, whereby unwanted heat is changed to useful electrical energy with no harmful emissions compared to other traditional power plants [1, 2]. The performance of a TE materials can be evaluated by the figure of merit, zT = S2σT/κ, where
To date, many innovative TE materials like Bi2Te3, PbTe, CoSb3 XNiSn, and SiGe have been commercially applied because of their high performance as compared to other TE materials [5, 8, 9, 10, 11, 12]. However, these materials have restricted applications due to their high price, instability in oxidizing atmospheres, and the most important toxicity [8, 13, 14, 15]. Therefore, many studies on alternative TE materials with low cost, high efficiency, and environmentally friendly characteristics have been explored [16, 17, 18]. In this relay, oxide materials have been considered as the best alternative, such as layered cobalt oxide (NaCo2O4), and strontium titanium oxide (SrTiO3) due to their low price, thermal stability, and eco-friendly compatibility [19, 20]. For TE applications,
Layered structure
Similar to highly studied NaCoO2 TE material, LiNbO2 has a layered configuration in which the NbO6 trigonal-prismatic layers and Li planes are stacked, as shown in the schematic Figure 1(a). This similarity proposes that LiNbO2 could be a new promising TE material. LiNbO2 is a sub-oxide of the main (LiNbO3), and its Li-intercalated structure Li1-
Stoichiometric SrTiO3 has a cubic perovskite structure, where oxygen anions form an octahedron with one Ti4+ atom lying at the center as shown in the schematic Figure 1(b). SrTiO3 have been studied widely and is considered as one of the favorite
Considering the importance of defects in oxide materials as discussed above, it is important to study cation and anion defect engineering in oxide materials. Here in this chapter we have considered LiNbO2 (
2. Cation defect engineering
2.1 Experimental and computational approaches
2.1.1 Preparation of Li1-x NbO2 compounds
Nonstiochiometric Li1-
2.1.2 Theoretical calculations of Li1-x NbO2
The electronic structures of Li1-
2.1.3 Characterization of Li1-x NbO2
X-ray diffraction (XRD) analysis was performed by Rigaku D/MAX-2500/PC with Cu K
2.2 Results and discussion
Figure 2(a) displays the XRD patterns of all samples. The main peaks of the compounds were indexed according to the LiNbO2 hexagonal structure which can be regarded as alternatively arranged close-packed Li-layers inserted among the two O-Nb-O slabs along the c-axis [29]. In addition to the main peaks, all samples showed small impurity peaks of LiNbO3 and NbO2. LiNbO3 peaks are expected due to moderate PO2 level during the consolidation process, which changes the oxidation state from Nb3+ to Nb5+. The additional NbO2 peaks can be described by the following defect reaction (1).
At lower Li-vacancy concentrations, the Li atoms to combine with Nb3+ ([1/3Nb5++2/3Nb2+]3+) make LiNbO2. But, at high Li-vacancy concentrations, there are insufficient Li-atoms to react with Nb3+ ([1/3Nb5++2/3Nb2+]3+) atoms to form LiNbO2 which turn into the NbO2 phase. Furthermore, at lower oxygen partial pressure the Nb5+ in the Li3NbO4 compound is thermally reduced to Nb4+ which is the consequence of the NbO2 phase. Additionally, the Li-vacancies lead to an increase in the repulsive force among the two adjacent oxygen layers which increases the
Figure 2(b)–(f) displays the fractured cross-section of Li1-
Figure 3(a) shows the temperature-dependent electrical conductivities of Li1-
To deeply understand the above experimental results DFT calculations were also employed and the electronic structures were calculated. The calculated electronic structure suggests that virgin LiNbO2 has a band-gap of 1.65 eV. It should be noted that DFT-LDA generally miscalculates the band-gap. But, the calculated band-gap in our work is consistent with the reported works [45]. Figure 3(b) summarizes the electronic DOS for various holes concentrations. It suggests that virgin LiNbO2 is a semiconductor and suggesting a metallic behavior for holes incorporated samples. Besides, the DOS at the Fermi energy also increases, suggesting that the electrical conductivity of Li1-
Figure 4(a) shows the temperature-dependent Seebeck coefficients (
Figure 4(b)–(d) shows the temperature-dependent Hall measurements for all Li1-
Figure 5(a) represents the temperature-dependent total thermal conductivities (
The figure-of-merit (zT) for all Li1-
3. Anion defect engineering
3.1 Experimental and computational methods
3.1.1 Preparation of SrTiO3-δ
Pristine SrTiO3 samples were synthesized by using conventional solid-state reaction techniques, using TiO2 and SrCO3 with a purity level higher than 99.9%. The stoichiometric powders were ball-milled for 24 hr. Next, the ball-milled powders were calcined at 1373 K for 3 hrs. The powders were then sieved and pressed into thicknesses of 3 mm. The pressed pellets were sintered at 1573 K for 30 hrs under the air atmosphere. To create an Anion defect in SrTiO3 (Oxygen vacancies), the samples were annealed by allowing 1%H2/Ar, 5%H2/Ar, 10%H2/Ar, and 20%H2/Ar gases at 1573 K for 30 hrs, and the samples were designated with the prefix “1HAr, 5HAr, 10HAr, and 20HAr”, respectively.
3.1.2 Theoretical calculations of SrTiO3-δ
To understand the anion defect engineering in SrTiO3, DFT with the local density approximations were applied and correlated with experimental work [44, 56]. To properly pronounce the electronic band structures of pristine and O-vacancies in SrTiO3, we also considered the LDA + U methodology by selecting the effective on-site Coulomb modification (U = 5.0 eV) is applied to d-orbital electrons in Ti-atom in agreement with the reported works [57, 58]. To compute the oxygen vacancy in SrTiO3, a 2 × 2 × 2 supercell was considered and the BoltzTraP program was used for TE properties [45, 46].
3.1.3 Charascterization of SrTiO3-δ
For SrTiO3-δ characterizations, the same techniques were followed as described in section 2.1.3.
3.2 Results and discussion
Figure 7 shows the XRD pattern of the reduced SrTiO3-
Sample | Lattice parameter (Å) | Carrier concentration (×1019 cm−3) | Oxygen vacancies (×1019 cm−3) | Mobility (cm2V−1 s−1) | Estimated (atm) |
---|---|---|---|---|---|
[1HAr] | 3.8991 | 0.106 | 0.0530 | 6.316 | 2.24 × 10−11 |
[5HAr] | 3.8999 | 0.198 | 0.099 | 5.373 | 7.78 × 10−15 |
[10HAr] | 3.9012 | 5.24 | 2.62 | 4.885 | 2.23 × 10−23 |
[20HAr] | 3.9047 | 10.660 | 5.33 | 3.694 | 3.17 × 10−25 |
Figure 8 shows the microstructure of thermally etched SrTiO3-
Figure 9 displays the high-resolution transmission electron microscopy (HRTEM) of oxygen-deficient SrTiO3-
Annealing under a reducing atmosphere at ambient temperature leads to different kinds of defects in materials. Oxygen vacancies could be one of the main defects in the SrTiO3 due to the low formation-energy compared to other atoms in the lattice. Below Eq. (6) shows in the Kröger-Vink notation [62].
where
where ∆
The observed carrier concentrations in our samples are in the range of 1018 to 1020/cm3, which is a typical range for Mott transition, i.e., insulator–metal transition. This transition can be calculated from the Mott criterion,
The temperature-dependent electrical conductivity and Seebeck coefficient of reduced SrTiO3-
DFT calculations were also used to understand the effect of O-vacancies in SrTiO3. The electronic band structures of virgin and O-deficient SrTiO3 samples were calculated using DFT + U, and the results are presented in Figure 10(c). Our DFT + U calculated electronic band-gap results suggest that of virgin SrTiO3 at Г-point is 2.31 eV (1.93 eV), which is close reported work [34, 66]. However, in the case of oxygen-deficient SrTiO3, the electronic band-gap is reduced to 2.18 eV at Г-point. The band structure calculations show a band below the conduction band, and an electron pocket which can be seen at the Г- point. Such an electronic pocket suggests electrons in the conduction band, which is largely formed by the Ti-
where
Figure 12(a) represents the temperature-dependent thermal conductivity of SrTiO3-
Figure 12(c) illustrates the temperature-dependent PF for various oxygen-deficient SrTiO3 samples. The substantial enhancement in the PF is due to the combination of moderate Seebeck coefficient values and high electrical conductivity. The PF obtained in this work is comparable to the PF obtained in doped-SrTiO3 [65]. The DFT calculated PF for various carrier concentrations (1018–1022/cm3) suggests that the highly reduced SrTiO3 samples would have higher PF as shown in Figure 12(d) [68]. Additionally, one of the most remarkable features of this study is the decoupling among electrical and thermal conductivity of SrTiO3-
Table 2 shows that the efforts in the layer-structured cobaltites and SrTiO3 based materials. It shows that significant improvements have been achieved in oxide TE materials, which could be of great interest for power generation applications at high operating temperatures. As compared with other oxides, the materials investigated in this study show relatively low figure of merit (zT), which is because the investigated Li1-xNbO2 and SrTiO3-δ are pure, undoped materials to understand the mechanism for cation and anion defects effects.
3.3 Conclusion
In conclusion, this work demonstrated that cation and anion vacancies can successfully control the thermoelectric performance of oxide-based thermoelectric materials. These findings suggest that both cation defect and anion defect can be engineered by reducing atmospheres and the defects in oxide thermoelectric materials simultaneously act as a source of charge carriers and phonon scattering centers. This decoupled behavior between electrical conductivity and thermal conductivity can lead to a substantial increase in the thermoelectric performance of oxide materials. The concept applied in this work is generally important and has the possibility of impacting the thermoelectric performance of oxide thermoelectrics and other functional oxide materials.
Acknowledgments
The experimental work was conducted by using the facilities in the Korea Institute of Ceramic Engineering and Technology (KICET). The authors, Jamil Ur Rahman and Soonil Lee are grateful to all colleagues for help and support in the same research group at KICET.
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