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Investigation of electrical properties and PTCR effect in double-donor doping BaTiO3 lead-free ceramics

  • Xiaoming Chen , Yini Li , Sikang Zeng , Xuxin Cheng EMAIL logo , Wei Zhang and Yuxin Wang
Published/Copyright: January 31, 2024
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High Temperature Materials and Processes
From the journal High Temperature Materials and Processes Volume 43 Issue 1

Abstract

Utilizing the conventional approach, the positive temperature coefficient of resistivity (PTCR) performance of lead-free ceramics based on (1 − x%)(Ba1−y Y y )(Ti1.011−z Nb0.001Mn z )O3 − x%(Bi0.5Na0.5)TiO3 (BBNTx) was examined. The BBNTx ceramics were prepared using the double donor dopant under firing at 1,350°C for 120 min in the air. The findings exhibited that when the Y3+ concentration elevates, the room-temperature resistivity of 99%(Ba1−y Y y )(Ti1.011−z Nb0.001Mn z )O3 – 1%(Bi0.5Na0.5)TiO3 (BBNT1) samples initially falls and subsequently elevates. Moreover, the critical content of the samples is 0.15 mol%. Furthermore, the samples’ resistance jumping ratio can be effectively improved by adding Mn2+. The manganese dioxide level of 0.05 mol% yields the greatest resistance-jumping ratio. Besides, the impact of (Bi0.5Na0.5)TiO3 (BNT) concentration on ceramics’ Curie temperature was examined in the work. Therefore, good free-lead PTCR thermistors were successfully prepared by doping 3% BNT, with a resistance jump of 4.1 magnitude.

Keywords: BaTiO3 ; Y2O3-dopant; PTCR effect; electroceramics

1 Introduction

A ferroelectric substance known as barium titanate (BaTiO3) is doped with trace amounts of pentavalent or trivalent donors (Nb5+, Sm3+, Y3+, and so on). It is a semiconducting material that reveals an amazing rise in resistance when it gets close to the Curie temperature [1,2]. The effect of positive temperature coefficient of resistivity (PTCR) is the name given to this phenomenon, which has been satisfactorily described by both Heywang [3] and Jonker [4]. During the past several years, the market for PTCR thermistors of the high temperature [5] that can be used in self-controlled heaters has grown. The lead titanate is usually doped in the samples to improve the ceramics’ Curie temperature. However, the lead is toxic. Recently, the compounds of (Bi1/2Na1/2) TiO3 (BNT) [6,7] along with (Bi1/2K1/2)TiO3 (BKT) [6,7] were doped to create lead-free PTCR ceramics. The Nb5+, Y3+, Mn2+, and BNT content as well as their impact on the PTCR effect and electrical characteristics of the lead-free ceramics based on BBNTx however have received less attention. Thus, this research explores the impact of the double-donor dopant on the PTCR properties of BBNTx ceramics.

2 Materials and methods

The raw components were high-purity NaCO3 (>99.8%), Bi2O3 (>99.8%), BaCO3 (>99.8%), Nb2O5 (>99.99%), Y2O3 (>99.99%), Mn(NO3)2 (>99.5%), and TiO2 (>99.8%), which were weighed according to the formula: (1 − x%)(Ba1−y Y y )(Ti1.011−z Nb0.001Mn z )O3 − x%(Bi0.5Na0.5)TiO3 (BBNTx). In our experiment, the concentration of x, y, z is in the range of 1–5 mol, 0.05–0.25 mol%, 0.03–0.09 mol%, respectively. First, the mixture of x%(Bi0.5Na0.5)TiO3 (BNTx) was combined by wet ball milling in alcohol for 4 h with an agate ball in a ninon jar, and lather was dried in a 90°C drying oven, and the powders were calcined for 120 min at 900°C in air. Second, an agate ball in a ninon jar was applied to a wet ball mill with the combination of (1 − x%)(Ba1−y Y y )(Ti1.011−z Nb0.001Mn z )O3 for 4 h in alcohol. The powders were next dried at 90°C in a drying oven and calcined for 120 min at 1,100°C in air. These mixtures were all reground for 6 h using a ball mill. To create the green compacts, which have a size of 15 mm × 2 mm, the dried powders were combined with 5 wt% polyvinyl alcohol and compressed at 150 MPa. After that, the blocks were sintered in an air muffle furnace for 120 min at 1,350°C, with a 250°C·h−1 heating rate, and furnace cooling was utilized for cooling. After applying Ag–Zn alloy to the fired BBNTx ceramic surfaces, they were sintered at 540°C for 10 min to generate electrodes. A digital multimeter was subsequently utilized to measure the specimens’ resistance at room-temperature (RT), and a temperature-programmable furnace (ZW-1, Huazhong University of Science and Technology, China) was employed to measure the resistance’s temperature dependence at 1.6 °C·min−1 heating rate between 25 and 250°C. Furthermore, scanning electron microscopy (SEM; Quanta FEG 250 FEI, American) was used to observe the surface microstructure of sintered ceramics. The line-intersection technique was applied to estimate the ceramics’ average grain size.

3 Results and discussion

3.1 Microstructure of the ceramics

The concentration of BNT has a major impact on the samples’ microstructure (Figure 1), and a discernible variation in grain size is seen. As concentrations of BNT rise, it slightly declines and becomes uniform, most likely as a result of decreased porosity as BNT content elevates. Consequently, variations in the rates of grain development might be the cause of the particle-size distribution. Cooling the liquid phase between 1,200 and 800°C allows it to solidify, and the higher the BNT concentration, the slower the mass-transfer and grain boundary movement processes become.

Figure 1 SEM micrograph on the surfaces of the BBNTx specimens sintered at 1350°C for 2 h with doping different BNT contents: (a) 1 mol%, (b) 2 mol%, (c) 3 mol%, and (d) 4 mol%.
Figure 1

SEM micrograph on the surfaces of the BBNTx specimens sintered at 1350°C for 2 h with doping different BNT contents: (a) 1 mol%, (b) 2 mol%, (c) 3 mol%, and (d) 4 mol%.

3.2 Impact of the double-donor dopant concentration on PTCR influence

Based on the resistance jump (Log10[R max/R min]) and RT resistivity of the 99%(Ba1−y Y y )(Ti1.011−z Nb0.001Mn z )O3 − 1%(Bi0.5Na0.5)TiO3 (BBNT1) (z = 0.05 mol%) ceramics, fired in the air at 1,350°C for 120 min, Figure 2 displays the impact of the dopant concentration on the PTCR influence, and the dopant content is presented in Figure 3, where R max and R min are the max and min resistance of the samples between RT and 250°C, respectively. Based on the figures, as the dopant concentration elevates, the ceramics’ RT resistivity initially lowers and subsequently increases. Conversely, a resistance jump displays a reverse tendency. This behavior indicates that 0.15 mol% Y3+ is the ideal donor-doped level. The resistivity leap raises with reducing RT resistivity. Moreover, the electrical compensation of the substituted Ti4+ and Ba2+ by the Nb5+ and Y3+, separately, is mostly responsible for the resistivity drop [8,9]:

(1) Y 2 O 3 → 2 Y Ba ˙ + 2 O O + 1 / 2 O 2 + 2 e ′ ,

(2) 2 BaO + Nb 2 O 5 → 2 Ba Ba + 2 Nb Ti ˙ + 6 O O + 1 / 2 O 2 + 2 e ′ .

Figure 2 Temperature dependence of resistivity of the BBNT1 ceramics sintered at 1,350°C for 2 h in air.
Figure 2

Temperature dependence of resistivity of the BBNT1 ceramics sintered at 1,350°C for 2 h in air.

Figure 3 RT resistivity and the resistance jump of the BBNT1 ceramics as a function of the dopant concentration.
Figure 3

RT resistivity and the resistance jump of the BBNT1 ceramics as a function of the dopant concentration.

Conversely, the rise in resistivity is typically ascribed to the ionic compensation brought about by the co-generation of titanium and barium vacancies [10,11]

(3) Y 2 O 3 → 2 Y Ba ˙ + V Ba ″ + 3 O O ,

(4) 5 BaO + 2 Nb 2 O 5 → 5 Ba Ba + 4 Nb Ti ˙ + V Ti ″ ″ + 15 O O .

3.3 Impact of doping Mn concentration on electrical performance

The resistance jump and RT resistivity of the BBNT1 (y = 0.15 mol%) samples that are fired at a temperature of 1,350°C for 120 min are shown in Figure 4. These electrical properties are affected by the Mn(NO3)2 concentration in the range of 0.03–0.09 mol%, and the effect of the manganese nitrate concentration on the PTCR performance is shown in Figure 5. From Figure 4, as the concentration of Mn rises, the RT resistivity of the ceramics elevates rapidly. Furthermore, when the Mn concentration of the ceramics rises, it initially elevates and subsequently falls. The Mn2+ level of 0.05 mol%, which is revealed by 3.1 orders of magnitude and possesses an RT resistivity of 2.9 × 103 Ω·cm, yields the ideal resistance jump. The outcome suggests that the specimens’ PTCR properties can be enhanced by a modest dose of Mn(NO3)2.

Figure 4 RT resistivity and the resistance jump of the BBNT1 ceramics as a function of the Mn(NO3)2 concentration.
Figure 4

RT resistivity and the resistance jump of the BBNT1 ceramics as a function of the Mn(NO3)2 concentration.

Figure 5 Temperature dependence of resistivity of the BBNT1 ceramics for different Mn(NO3)2 content sintered at 1,350°C for 2 h in air.
Figure 5

Temperature dependence of resistivity of the BBNT1 ceramics for different Mn(NO3)2 content sintered at 1,350°C for 2 h in air.

The impact of the electrical performances of the BBNTx (y = 0.15 mol%, z = 0.05 mol%) ceramics, which were sintered at a temperature of 1,350°C for 120 min, is shown in Figure 6. The impact of varying concentrations of BNT on the PTCR effect of ceramics in Figure 6 is illustrated in Figure 7 – the BBNTx samples with doping 1, 2, 3, and 4 mol% BNT. The figures demonstrate that when the BNT concentration rises, so does the specimens’ RT resistivity. Conversely, the jumping ratio of ceramics first increases very slightly and later decreases rapidly with increasing BNT concentrations. Therefore, with an RT resistivity of 7.2 ×103 Ω·cm in Table 1, the best PTCR effect under the BNT concentration is 3 mol%, which is revealed by 4.1 orders of magnitude. Usually, the ionic compensation brought about by the creation of cation vacancies is accounted for by the rise in resistivity.

Figure 6 RT resistivity and the jumping ratio of the BBNTx ceramics as a function of the BNT content.
Figure 6

RT resistivity and the jumping ratio of the BBNTx ceramics as a function of the BNT content.

Figure 7 Temperature dependence of resistivity of the BBNTx samples sintered at 1,350°C for 2 h in air.
Figure 7

Temperature dependence of resistivity of the BBNTx samples sintered at 1,350°C for 2 h in air.

Table 1

Electrical properties and PTCR effect of the BBNTx samples fired at 1,350°C for 2 h in air

Electrical properties Samples
BNT1 BNT2 BNT3 BNT4 BNT5
ρ (Ω·cm) 3.0 × 103 4.3 × 103 7.2 × 103 1.4 × 105 1.6 × 106
Lg(R max/R min) 3.1 2.1 4.1 2.4 0.7
T c (°C) 137 143 147 150 154

4 Conclusion

Resistance jump and electrical characteristics of the BBNTx ceramics sintered in the air at 1,350°C for 120 min were examined in the article. The findings suggested that when the amount of Y dopant in BBNT1 ceramics rises, the RT resistivity initially reduces and subsequently elevates. However, a resistance jump shows a contrary tendency. Consequently, 0.15 mol% Y3+ is the critical donor-doped concentration. Furthermore, when the BNT and Mn level elevates, so does the samples’ RT resistivity. The manganese nitrate level of 0.05 mol% yields the best resistance jumping ratio. Moreover, the BNT concentration influences the PTCR properties of the ceramics. With an RT resistivity of 7.2 × 103 Ω·cm, the optimal PTCR effect is achieved at a doping BNT concentration of 3 mol%, as demonstrated by 4.1 orders of magnitude.

  1. Funding information: This study was funded by the National Natural Science Foundation of China (No. 51402258), the Key Research Platform and Program in Universities under the Department of Education of Guangdong Province (No. 2020GCZX003), the State Key Laboratory of Advanced Materials and Electronic Components (No. FHR-JS-202011007), the Research Laboratory of University Physics Course in Universities of Department of Education of Guangdong Province, the Fourth Batch of Innovative Research Teams at Zhaoqing University (TD202412), and the Quality Engineering Project in Zhaoqing University (No. zlgc202116).

  2. Author contributions: Xiaoming Chen: writing – original draft, Yini Li: writing – review and editing, Sikang Zeng: writing – original draft; Xuxin Cheng: writing – review and methodology; Wei Zhang: writing – review and editing; Yuxin Wang: writing – review and methodology.

  3. Conflict of interest: The authors state no conflict of interest.

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Received: 2024-04-22
Revised: 2024-08-15
Accepted: 2024-08-25
Published Online: 2024-01-31

© 2024 the author(s), published by De Gruyter

This work is licensed under the Creative Commons Attribution 4.0 International License.

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https://doi.org/10.1515/htmp-2024-0064
Keywords for this article
BaTiO3; Y2O3-dopant; PTCR effect; electroceramics
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  71. Investigation of the interface and physical properties of a Kovar alloy/Cu composite wire processed by multi-pass drawing
  72. The investigation of peritectic solidification of high nitrogen stainless steels by in-situ observation
  73. Microstructure and mechanical properties of submerged arc welded medium-thickness Q690qE high-strength steel plate joints
  74. Experimental study on the effect of the riveting process on the bending resistance of beams composed of galvanized Q235 steel
  75. Density functional theory study of Mg–Ho intermetallic phases
  76. Investigation of electrical properties and PTCR effect in double-donor doping BaTiO3 lead-free ceramics
  77. Special Issue on Thermal Management and Heat Transfer
  78. On the thermal performance of a three-dimensional cross-ternary hybrid nanofluid over a wedge using a Bayesian regularization neural network approach
  79. Time dependent model to analyze the magnetic refrigeration performance of gadolinium near the room temperature
  80. Heat transfer characteristics in a non-Newtonian (Williamson) hybrid nanofluid with Hall and convective boundary effects
  81. Computational role of homogeneous–heterogeneous chemical reactions and a mixed convective ternary hybrid nanofluid in a vertical porous microchannel
  82. Thermal conductivity evaluation of magnetized non-Newtonian nanofluid and dusty particles with thermal radiation
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