All Issue

2025 Vol.35, Issue 9 Preview Page

Research Paper

Low-Temperature Sintering and the Dielectric Properties of the Lead Lanthanum Zirconate Titanate Ceramics According to Additives

첨가제에 따른 PLZT 세라믹스의 저온 소결과 유전특성

Yong Geun Choi1
,
Jeoung Sik Choi2
,
Hyo Soon Shin1†
,
Dong Hun Yeo1
,
Young Jin Lee1
최 용근1
,
최 정식2
,
신 효순1†
,
여 동훈1
,
이 영진1
1AI Convergence R&D Group, Korea Institute of Ceramic Engineering and Technology, Jinju 52851, Republic of Korea
2Pusan National University Technology Holdings, Busan 46241, Republic of Korea
1한국세라믹기술원
2부산대학교기술지주
†Corresponding author E-Mail : hshin@kicet.re.kr (H. S. Shin, KICET)
27 September 2025. pp. 428-435
PDF XML Citation
Abstract

Interest in high-permittivity dielectric materials suitable for classical systems has been increasing, and competition for commercial applications continues. However, despite the development of such dielectric materials, additional compositional improvements are still required to achieve low-temperature sintering that would allow co-firing with Cu internal electrodes in multilayer structures, and research in this area remains insufficient. In this study, we aimed to optimize a low-temperature sintering composition based on Pb0.94La0.06(Zr0.83Ti0.17)O3, which, in preliminary experiments, exhibited a dielectric constant above 1,300 at sintering temperatures exceeding 1300 °C. As the amount of Na ion addition increased, low-temperature sintering was effectively promoted. However, the dielectric constant simultaneously decreased. When K ions were further added to the Lead Lanthanum Zirconate Titanate (PLZT)+Na composition, the low-temperature sintering properties were maintained or improved, and the dielectric constant increased compared with Na-only addition. To precisely readjust the MPB region under the influence of large additive content, the Zr ion fraction was varied from 0.84 to 0.92. Within this range, the MPB composition was found to shift slightly as the Zr content increased. As a result, the optimal composition among the PLZT ceramics sintered at 950 °C was determined to be Zr 0.86, which exhibited a dielectric constant of approximately 900 and an energy storage density of about 2 J/cm3. These findings suggest that such a composition could be applicable for low-temperature co-firing with Cu electrodes in Multi-Layer Ceramic Capacitors (MLCCs) for classical systems.

Keywords
low temperature sintering
Lead Lanthanum Zirconate Titanate (PLZT)
anti-ferroelectric
dielectric constant
additives
References
1

T. Badapanda, S. Sahoo and P. Nayak, IOP Conf. Ser.: Mater. Sci. Eng., 178, 012032 (2017).

10.1088/1757-899X/178/1/012032
2

R. Rianyoi, R. Potong, N. Jaitanong, R. Yimnirun and A. Chaipanich, Appl. Phys. A, 104, 661 (2011).

10.1007/s00339-011-6307-2
3

J. Xie, L. Li, M. Wang and K. Xue, Mater. Chem. Phys., 277, 125 (2021).

4

L. Chen, H. Wang, P. Zhao, Z. Shen, C. Zhu, Z. Cen, L. Li and X. Wang, J. Am. Ceram. Soc., 102, 2781 (2019).

5

A. Chauhan, S. Patel, R. Vaish and C. R. Bowen, Materials., 8, 8009 (2015).

10.3390/ma812543928793694PMC5458845
6

F. Gao, X. Dong, C. Mao, W. Liu, H. Zhang, L. Yang, F. Gao and G. Wang, J. Am. Ceram. Soc., 94, 4382 (2011).

7

S. Jiang, L. Zhang, G. Zhang, S. Liu, J. Yi, X. Xiong, Y. Yu, J. He and Y. Zeng, Ceram. Int., 39, 5571 (2013).

10.1016/j.ceramint.2012.12.071
8

A. Peláiz-Barranco, J. D. S. Guerra, O. García-Zaldívar, F. Calderón-Piñar, M. E. Mendoza, D. A. Hall and E. B. Araújo, Solid. State. Commun, 149, 1308 (2009).

10.1016/j.ssc.2009.05.004
9

Z. Ujma, J. Handerek, M. Pawelczyk, H. Hassan, G. E. Kugel and C. Carabatos-Nedelec, J. Phys.:Condens. Matter, 6, 6843 (1994).

10.1088/0953-8984/6/34/016
10

G. H. Maher, J. Am. Ceram. Soc., 66, 408 (1983).

11

X. Hao, J. Zhou and S. An, J. Am. Ceram. Soc., 94, 1647 (2011).

12

T. R. Gururaja and E. C. Subbarao, Ferroelectrics., 23, 101 (1980).

10.1080/00150198008224816
13

S.-Y. Chu, T.-Y. Chen, I.-T. Tsai and W. Water, Sens. Actuators. A. Phys., 113, 198 (2004).

10.1016/j.sna.2004.02.020
14

D. Dong, K. Murakami, S. Kaneko and M. Xiong, J. Ceram. Soc. Jpn., 101, 1090 (1993)

10.2109/jcersj.101.1090
15

R. Zuo, L. Li, Z. Gu, X. Hu and C. Ji, J. Am. Ceram. Soc., 85, 787 (2004).

16

N. Horchidan, C. E. Ciomaga, R. C. Frunza, C. Capiani, C. Galassi and L. Mitoseriu, Ceram. Int., 42, 9125 (2016).

10.1016/j.ceramint.2016.02.179
17

L. Eyraud, P. Eyraud, L. Lebrun, B. Guiffard, E. Boucher, D. Audigier and D. Guyomar, Ferroelectrics., 265, 303 (2002).

10.1080/00150190208260631
18

J.-W. Li, Y.-X. Liu, H.-C. Thong, Z. Du, Z. Li, Z.-X. Zhu, J.-K. Nie, J.-F. Geng, W. Gong and K. Wang, J. Alloys. Compd., 847, 155936 (2020).

10.1016/j.jallcom.2020.155936
19

W. K. Lin, Y. H. Chong, Mater. Sci. Eng. A., 186, 177 (1994).

20

J.-S. Choi, D.-C. Kim, H.-S. Shin, D.-H. Yeo and J.-H. Lee, Appl, Sci., 12, 2591 (2022).

10.3390/app12052591
21

M. Oldenkotte, H. Kungl, R.-A. Eichel, K. A. Schönau, M. Kühlein, T. Bernard, M. J. Hoffmann and M. Hinterstein, J. Am. Ceram. Soc., 102, 5401 (2019).

10.1111/jace.16417
22

D. Northrop, J. Am. Ceram. Soc., 50, 441 (1967).

23

E. Kang and J. H. Park, New Phys.: Sae Mulli, 74, 664 (2024)

10.3938/NPSM.74.664
24

X. Qiao, H. Zhang, T. Guo, W. Geng and X. Chou, ACS OMEGA, 9, 5780 (2024).

10.1021/acsomega.3c0860738343983PMC10851414
25

A. Limpichaipanit and A. Ngamjarurojana, Actuators, 12, 74 (2023).

10.3390/act12020074
26

A. Limpichaipanit and A. Ngamjarurojana, Ceram. Int., 43, 4450 (2017).

10.1016/j.ceramint.2016.12.094
27

A. Limpichaipanit and A. Ngamjarurojana, Ferroelectrics., 486, 57 (2015).

10.1080/00150193.2015.1100025
28

H. R. Rukmini, R. N. P. Choudhary and D. L. Prabhakara, Mater. Chem. Phys., 64, 171 (2000).

10.1016/S0254-0584(99)00149-2
29

D. L. Corker, R. W. Whatmore, E. Ringgaard and W. W. Wolny, J. Eur. Ceram. Soc., 20, 2039 (2000).

10.1016/S0955-2219(00)00089-3
30

S. Dutta, R. N. P. Choudhary and P. K. Sinha, Mater. Sci. Eng. B, 113, 215 (2004).

10.1016/j.mseb.2004.08.006
31

D. K. Mahato and R. K. Chaudhary, J. Mater. Sci. Lett., 22, 1615 (2003).

10.1023/A:1026396710879
32

D. Damjanovic, Rep. Prog. Phys., 61, 1267 (1998).

10.1088/0034-4885/61/9/002
33

G. Arlt, D. Hennings and G. De, J. Appl. Phys., 58, 1619 (1985).

10.1063/1.336051
34

N. Setter and L. E. Cross, J. Mater. Sci., 15, 2478 (1980).

10.1007/BF00550750
35

S. Zhang and F. Li, J. Appl. Phys., 111, 031301 (2012).

36

H. R. Rukmini, R. N. P. Choudhary and V. V. Rao, J. Mater. Sci., 34, 4815 (1999).

37

A. Kumar, A. K. Kalyani, R. Ranjan, K. C. J. Raju, J. Ryu, N. Park and A. R. James, J. Alloys. Compd., 816, 152613 (2020).

10.1016/j.jallcom.2019.152613
38

K. Ramam and K. Chandramouli, Ceram.-Silikáty, 53, 189 (2009).

39

Y. Zhao, X. Hao and Q. Zhang, ACS. Appl. Mater. Interfaces., 6, 11633 (2014).

10.1021/am405014f
40

Z. Hu, B. Ma, S. Liu, M. Narayanan and U. Balachandran, Ceram. Int., 40, 557 (2014).

10.1016/j.ceramint.2013.05.139
41

G. Hu, C. Ma, W. Wei, Z. Sun, L. Lu, S.-B. Mi, M. Liu, B. Ma, J. Wu and C.-L. Jia, Appl. Phys. Lett., 109, 193904 (2016).

Information
  • Publisher :Materials Research Society of Korea
  • Publisher(Ko) :한국재료학회
  • Journal Title :Korean Journal of Materials Research
  • Journal Title(Ko) :한국재료학회지
  • Volume : 35
  • No :9
  • Pages :428-435
  • Received Date : 2025-09-02
  • Revised Date : 2025-09-11
  • Accepted Date : 2025-09-11
  • DOI :https://doi.org/10.3740/MRSK.2025.35.9.428
Journal Informaiton Korean Journal of Materials Research Korean Journal of Materials Research
Online Submission
  • scopus
  • NRF
  • KOFST
  • crossref crossmark
  • crossref cited-by
  • crosscheck
  • open access
  • ccl
Journal Informaiton Journal Informaiton - close