AU2021103649A4 - Tuning sodium and oxygen mixed-ion conduction in the A-site nonstoichiometric NaNbO3-based ceramics - Google Patents
Tuning sodium and oxygen mixed-ion conduction in the A-site nonstoichiometric NaNbO3-based ceramics Download PDFInfo
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- 239000000919 ceramic Substances 0.000 title abstract description 17
- 239000011734 sodium Substances 0.000 title abstract description 10
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 title abstract 2
- 229910003378 NaNbO3 Inorganic materials 0.000 title abstract 2
- 229910052708 sodium Inorganic materials 0.000 title abstract 2
- MUPJWXCPTRQOKY-UHFFFAOYSA-N sodium;niobium(5+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Na+].[Nb+5] MUPJWXCPTRQOKY-UHFFFAOYSA-N 0.000 title abstract 2
- 239000001301 oxygen Substances 0.000 title description 12
- 229910052760 oxygen Inorganic materials 0.000 title description 12
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 title description 8
- 239000000463 material Substances 0.000 abstract description 16
- 239000013078 crystal Substances 0.000 abstract description 3
- 239000010416 ion conductor Substances 0.000 abstract description 3
- 230000007812 deficiency Effects 0.000 abstract description 2
- 238000006243 chemical reaction Methods 0.000 abstract 1
- RKTYLMNFRDHKIL-UHFFFAOYSA-N copper;5,10,15,20-tetraphenylporphyrin-22,24-diide Chemical compound [Cu+2].C1=CC(C(=C2C=CC([N-]2)=C(C=2C=CC=CC=2)C=2C=CC(N=2)=C(C=2C=CC=CC=2)C2=CC=C3[N-]2)C=2C=CC=CC=2)=NC1=C3C1=CC=CC=C1 RKTYLMNFRDHKIL-UHFFFAOYSA-N 0.000 abstract 1
- 238000012983 electrochemical energy storage Methods 0.000 abstract 1
- 239000011159 matrix material Substances 0.000 abstract 1
- 229910001251 solid state electrolyte alloy Inorganic materials 0.000 abstract 1
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 8
- 239000000843 powder Substances 0.000 description 8
- 238000000034 method Methods 0.000 description 6
- 238000002441 X-ray diffraction Methods 0.000 description 5
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 4
- 238000005259 measurement Methods 0.000 description 4
- -1 oxygen ion Chemical class 0.000 description 4
- 239000008188 pellet Substances 0.000 description 4
- 239000012071 phase Substances 0.000 description 4
- 230000007547 defect Effects 0.000 description 3
- 238000010438 heat treatment Methods 0.000 description 3
- 238000001566 impedance spectroscopy Methods 0.000 description 3
- 238000003746 solid phase reaction Methods 0.000 description 3
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 2
- 229910016523 CuKa Inorganic materials 0.000 description 2
- 238000000627 alternating current impedance spectroscopy Methods 0.000 description 2
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 2
- 238000001354 calcination Methods 0.000 description 2
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 2
- 239000000969 carrier Substances 0.000 description 2
- 238000012512 characterization method Methods 0.000 description 2
- 239000003153 chemical reaction reagent Substances 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 150000002500 ions Chemical class 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 238000000746 purification Methods 0.000 description 2
- 230000005855 radiation Effects 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- 238000005245 sintering Methods 0.000 description 2
- UYLYBEXRJGPQSH-UHFFFAOYSA-N sodium;oxido(dioxo)niobium Chemical compound [Na+].[O-][Nb](=O)=O UYLYBEXRJGPQSH-UHFFFAOYSA-N 0.000 description 2
- 238000010671 solid-state reaction Methods 0.000 description 2
- 230000007704 transition Effects 0.000 description 2
- 238000005303 weighing Methods 0.000 description 2
- 230000005536 Jahn Teller effect Effects 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000006399 behavior Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 150000001768 cations Chemical class 0.000 description 1
- 239000002800 charge carrier Substances 0.000 description 1
- 239000004020 conductor Substances 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 230000002950 deficient Effects 0.000 description 1
- 238000000157 electrochemical-induced impedance spectroscopy Methods 0.000 description 1
- 239000002001 electrolyte material Substances 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 230000001699 photocatalysis Effects 0.000 description 1
- 238000009877 rendering Methods 0.000 description 1
- 239000006104 solid solution Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
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- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
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Abstract
:
Associations of two mobile ionic species (positive and the other
negative charges) in a specific matrix as solid-state electrolytes are of
high interest in electrochemical energy storage and conversion devices.
Here a strategy of A-site nonstoichiometric ratio was applied in
NaNbO3-based ceramics. The crystal structure, microstructure, and
electric properties of NaNbO 3-based ceramic (0.96NaxNbO 3-0.04CaZrO 3,
x = 0.96 to 1.02 mol %) was investigated. The P21ma phase was
maintained for all samples and the grain size increased from 5.72 pm to
8.93 pm with increasing the Na content. The conductance mode presented
3 different types with the various sodium contents: In the case of Na
deficiency, the Na+ and 02- mixed-ion conductance was appeared. At
lower temperature (400 °C-540 °C), Na+ was the main carrier. When the
temperature up to 540 °C, the crystal structure transformed to tetragonal
phase, and the main carrier changed from Na+ to 02- (Type I). The
stoichiometric sample was an ionic conductor with Na+ as the main
carrier (Type II). Moreover, the samples with excess Na were ionic
conductivity materials with 02- as the main carrier (Type III). This work
provides a new strategy to tune the mixed ionic conductivity of
NaNbO 3-basedceramics.
Description
1. Background and Purpose
Sodium niobate (NaNbO 3 ) and its related perovskites have attracted considerable
attention due to their unique combination of superior electrical and mechanical
properties. Upon variation of temperature, NaNbO 3 exhibits an unusually large
number of phase transitions, owing to tilted oxygen octahedral and off-centered Nb
ions, rendering it one of the most complicated perovskite materials from a structural
point of view. As a result, this group of materials is of interest from the tunability of
variously electrical properties.
In recent years, oxygen vacancy defects have been found in NaNbO 3 and used in
various fields. Yang et al. synthesized NaNbO 3 ceramics with oxygen vacancy defects
through a solid-phase reaction method. The oxygen vacancy defects resulted in a
larger specific surface area and charge density, which greatly increased its
photocatalytic performance. Besides, Gouget et al. prepared NaNbTix0 3o. 5x ceramic
material through a two-step synthesis process including hydrothermal and subsequent
heat treatment, which has high ionic conductivity between 300 °C and 700 °C. The
substitution of Ti for Nb atoms made it easier for sodium niobate to form the acentric
polymorph instead of the usual thermodynamically stable form (Pbma space group).
After Ti replaces Nb, a large change in the bond length of Nal - 01 and Na2 - 02
reduced the tip distortion of Nb/Ti-01 and Nb/Ti-02, thereby increasing the
equatorial plane distortion. The distortion of the larger Nb(Ti)0 6 octahedron enhanced
the second-order Jahn-Teller effect. Enhancement of the second-order Jahn-Teller
effect led to high oxygen mobility and lowers the phase transition temperature from
P21ma to Cmcm and from Cmcm to Pm-3m. And due to the low valence of Ti 4 *, there were a large number of oxygen vacancy defects in the material lattice, which greatly increased its oxygen ion conductivity. With the deepening of research, Gouget et al.
found that the Na+ conduction was presented in NaNbO 3. Nb5 - (4d0) and Ti 4 -based
(3d0) derived-perovskite frameworks containing Na+ and 02- as mobile species were
investigated as mixed ion conductors by electrochemical impedance spectroscopy. By
preparing Na+ barrier/0 2 - specific electrolyte materials on both sides of the material,
the 02- transmission amount was measured, and then the Na+ transmission number
was deduced. By preparing Na+ transport materials on both sides of the material, the
amount of Na+ transport and infer the amount of 02- transport was measured. In the
pure NaNbO 3, both Na+ (tNa+ = 88%) and 02- (t 0 2- = 12%, independent to temperature)
participated to the conductivity in a poor ion conductor. In the case of
NaNbo. 9Tio 0O 2 .95, the Na+ conductivity of the material gradually decreased with the
increase of temperature, and the 02- conductivity gradually increased, and starting at
350 °C, the Na+ conduction was completely suppressed, and the material became pure
02- conductor material.
The component, the tolerance factor, and the charge neutrality for solid solutions
or doped materials consider perovskite oxides as ionic crystals. From this point of
view, reducing the number of A-site cations will lead to the deficiency of positive
charge. In order to balance the charge, the negative charge oxygen anions must be
removed, thus forming charged oxygen vacancies. The absence of A-site also leads to
the corresponding vacancy, which result the increase of conductivity of A-site ions.
Based on the conclusions from above, NaNbO 3-based ceramics with different Na content and the effect of non-stoichiometric ratio on the electrical properties was investigated. The electrical properties of these non-stoichiometric NaNbO 3-based ceramics were established by a combination of impedance spectroscopy. Three different electrical behaviors were found in the nonstoichiometric NaNbO 3-based ceramics. For Na deficient samples, Na+ was the main charge carriers at low temperature. However, the 02- as the main carrier was emerged at high temperature
(Type I). For Na stoichiometric sample, Na+ was the main carriers. For Na excess
samples, 02- was the main carriers in the temperature range of 400-700 °C (Type III).
This work reveals the influence of A-site non stoichiometric ratio on the
microstructure and electrical properties of NaNbO 3-based ceramics and can provide
guidance for the selection of appropriate stoichiometric ratio to meet the electrical
properties requirements of the solid-state battery.
2. Experimental procedure
2.1. The procedures of materials preparation are as follows:
Step 1: Polycrystalline ceramics of 0.96NaxNbO 3-0.04CaZrO 3 (x =0.96, 0.98,
0.99, 1.0, 1.01 and 1.02) were prepared by a traditional solid-state reaction. Carbonate
NaCO 3 (99.9%), CaCO 3 (99.9%) and oxide Nb 2 05 (99.9%), ZrO2 (99.9%) were
purchased from Shanghai Aladdin Biochemical Technology Co., Ltd., CN and used
without further purification.
Step 2: The raw materials were dried in an oven at 180 °C for 8 h before
weighing to reduce hygroscopic carbonates. Accurately weigh these reagents
according to the molar ratio, and suspended it in ethanol and then milled in a planetary ball mill for 12 h using zirconia balls.
Step 3: The following calcination was conducted in a covered alumina crucible at
850 °C for 2 h. To guarantee a homogeneous distribution, the calcined powders were
ball milled again for 12 h. The prepared powders have been uniaxially compacted into
pellets (diameter 10 mm) with a pressure of ca. 25 MPa and pressed cold isostatically
at 200 MPa.
Step 4: Finally, the pressed pellets were covered with the same composition
powders and then sintered at 1250 ~ 1350 °C for 2 h at a heating rate of 4 °C/min.
2.2 The procedures of materials characterization are as follows:
Step 1: XRD patterns were recorded with a laboratory X-ray diffractometer (XRD,
D8ADVANCE, Brooke, Germany) using CuKa incident radiation (X = 1.54056 A) in
the 20 range of 10 ~ 80°. XRD patterns were collected on the powder obtained by
crushing the as-sintered samples.
Step 2: The surface morphologies of the ceramics were performed using a field
emission scanning electron microscope (SEM, SEM450, FEI Nova Nano, Czech
Republic).
Step 3: The working electrodes were manufactured by coating and sintering of
electronic paste. After sanding both sides of the ceramic sample into flat surface, Pt
electronic paste was coated on both sides of the ceramic sample and casted at room
temperature for 10 minutes. Finally, the prepared electrodes were sintered at 850 °C
for 15 min after drying at 100 °C. The dielectric properties of the samples were tested
in the temperature range 25 °C- 500 °C at different frequencies by using an LCR meter.
Step 4: AC impedance spectroscopy (IS) measurements were performed in
different atmosphere (02, air and N2) by using an electrochemical workstation
(CHI700e, CH Instruments Ins, China). The conductivity of oxygen ions is
determined by electromotive force (EMF) measurements, which were performed at
400 °C- 700 °C using 02, air and N 2 gases.
(1) The procedures of materials preparation are as follows:
Step 1: Polycrystalline ceramics of 0.96NaxNbO 3-0.04CaZrO 3 (x =0.96, 0.98,
0.99, 1.0, 1.01 and 1.02) were prepared by a traditional solid-state reaction. Carbonate
NaCO 3 (99.9%), CaCO 3 (99.9%) and oxide Nb 2 05 (99.9%), ZrO2 (99.9%) were
purchased from Shanghai Aladdin Biochemical Technology Co., Ltd., CN and used
without further purification.
Step 2: The raw materials were dried in an oven at 180 °C for 8 h before
weighing to reduce hygroscopic carbonates. Accurately weigh these reagents
according to the molar ratio, and suspended it in ethanol and then milled in a
planetary ball mill for 12 h using zirconia balls.
Step 3: The following calcination was conducted in a covered alumina crucible at
850 °C for 2 h. To guarantee a homogeneous distribution, the calcined powders were
ball milled again for 12 h. The prepared powders have been uniaxially compacted into
pellets (diameter 10 mm) with a pressure of ca. 25 MPa and pressed cold isostatically
at 200 MPa.
Step 4: Finally, the pressed pellets were covered with the same composition
powders and then sintered at 1250 ~ 1350 °C for 2 h at a heating rate of 4 °C/min.
(2) The procedures of materials characterization are as follows:
Step 1: XRD patterns were recorded with a laboratory X-ray diffractometer
(XRD, D8ADVANCE, Brooke, Germany) using CuKa incident radiation (X =
1.54056 A) in the 20 range of 10 ~ 80°. XRD patterns were collected on the powder obtained by crushing the as-sintered samples.
Step 2: The surface morphologies of the ceramics were performed using a field
emission scanning electron microscope (SEM, SEM450, FEI Nova Nano, Czech
Republic).
Step 3: The working electrodes were manufactured by coating and sintering of
electronic paste. After sanding both sides of the ceramic sample into flat surface, Pt
electronic paste was coated on both sides of the ceramic sample and casted at room
temperature for 10 minutes. Finally, the prepared electrodes were sintered at 850 °C
for 15 min after drying at 100 °C. The dielectric properties of the samples were tested
in the temperature range 25 °C- 500 °C at different frequencies by using an LCR
meter.
Step 4: AC impedance spectroscopy (IS) measurements were performed in
different atmosphere (02, air and N2) by using an electrochemical workstation
(CHI700e, CH Instruments Ins, China). The conductivity of oxygen ions is
determined by electromotive force (EMF) measurements, which were performed at
400 °C- 700 °C using 02, air and N 2 gases.
Fig. 1. (a) and (b) X-ray diffraction spectra of 0.96NaxNbO3-0.04CaZrO3 (x=0.96, 0.98, 0.99, 1,
1.01 and 1.02). (c) Rietveld profiles considering P21ma phases for the x = 0.96 sample. (d) and (e)
are lattice constants and unit cell volumes of P21ma phases with different contents of Na.
Fig. 2. (a) Nyquist plots of 0.96NaxNbO3-0.04CaZrO3 at 500 °C, (b) x=0.96 samples at different
temperatures, (c) Normalized DRT curves at different temperatures, and (d) the corresponding
Arrhenius diagram for x=0.96 samples.
Fig. 3. The Nyquist plots in different atmosphere (O2, air, and N2) and the corresponding
Arrhenius diagram, (a) and (b) for x=0.96 samples, (c) and (d) for x=1.0 samples, (e) and (f) for
x=1.02 samples.
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| CN115376825A (en) * | 2022-08-16 | 2022-11-22 | 中国科学院上海硅酸盐研究所 | NN-based energy storage ceramic block material with high energy storage density and energy storage efficiency and preparation method thereof |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115376825A (en) * | 2022-08-16 | 2022-11-22 | 中国科学院上海硅酸盐研究所 | NN-based energy storage ceramic block material with high energy storage density and energy storage efficiency and preparation method thereof |
| CN115376825B (en) * | 2022-08-16 | 2023-08-08 | 中国科学院上海硅酸盐研究所 | NN-based energy storage ceramic block material with high energy storage density and energy storage efficiency and preparation method thereof |
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