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通过两步固相反应烧结法制备了(1–x) Pb0.99Nb0.02[(Zr0.57Sn0.43)0.94Ti0.06]0.98O3:xAlN ((1–x)PNZST:xAlN, x = 0, 0.1, 0.2, 0.3, 0.4))复合陶瓷, 系统研究了复合陶瓷晶体结构、微观形貌、畴结构演变以及铁电、介电和热释电性能等. 实验结果表明: 基于两相之间热膨胀系数失配产生的局域应力场有效调控了畴结构组态和相结构演变, 在室温附近构建了铁电/反铁电相界, 继而在温度场作用下表现出优异的热释电性能; 当x = 0.1时, 在近人体温度37 ℃时其热释电系数p达到最大值3.30×10–3 C/(m2⋅K), 电流响应优值Fi = 3.16 × 10–9 m/V, 电压响应优值Fv = 0.613 m2/C, 探测率优值Fd = 4.40×10–4 Pa–1/2, 且其半峰宽为16.3 ℃, 在室温宽温域内表现出优异的热释电性能; 随着AlN含量的增多, 该复合陶瓷的热释电峰值温度在37—73 ℃宽温域内可调, 表现出良好的温度稳定性.In this work, composite ceramics (1–x)Pb0.99Nb0.02[(Zr0.57Sn0.43)0.94Ti0.06]0.98O3:xAlN (abbreviated (1–x)PNZST:xAlN, x = 0, 0.1, 0.2, 0.3 and 0.4) are prepared by a two-step solid phase synthesis method. The crystal structures, micromorphologies, domain structure evolutions, ferroelectric, dielectric and pyroelectric properties of those composite ceramics are systematically investigated. The results show that the difference in thermal expansion coefficient between PNZST and AlN creates compressive stresses in the PNZST matrix when cooling down from the sintering temperature, then a metastable ferroelectric (FE) phase is induced in the anti-FE matrix by the AlN component-induced internal stress, and in turn ferroelectric/antiferroelectric phase boundary is constructed near room temperature. As the temperature increases, the ferroelectric-to-antiferroelectric phase transition causes a larger pyroelectric current peak. In particular, the composition with x = 0.1 exhibits a high pyroelectric coefficient p = 3.3×10–3 C⋅m–2⋅K–1 and figure-of-merit with current responsivity Fi = 3.16×10–9 m⋅V–1, voltage responsivity Fv = 0.613 m2⋅C–1, and detectivity Fd = 4.4×10–4 Pa–1/2 around human body temperature. Moreover, the enhanced pyroelectric coefficient exists in a broad operation temperature range with a large full width at half maximums of 16.3 ℃ at 37 ℃. With the increase of AlN content, the pyroelectric peak temperature of the composite ceramic is adjustable in a wide temperature range of 37–73 ℃, showing good temperature stability.
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Keywords:
- pyroelectricity /
- composite ceramics /
- local stress field /
- ferroelectric domain
[1] Liu Z, Lu T, Dong X, Wang G, Liu Y 2021 IEEE Trans. Ultrason. Ferr. 68 242Google Scholar
[2] Jia J, Guo S, Yan S, Cao F, Yao C, Dong X, Wang G 2019 Appl. Phys. Lett. 114 032902Google Scholar
[3] Whatmore R W 1986 Rep. Prog. Phys. 49 1135Google Scholar
[4] Wang Y, Yuan G, Luo H, Li J, Viehland D 2017 Phys. Rev. Appl. 8 034032Google Scholar
[5] Domingo N, Bagués N, Santiso J, Catalan G 2015 Phys. Rev. B 91 094111Google Scholar
[6] Pandya S, Wilbur J, Kim J, Gao R, Dasgupta A, Dames C, Martin L W 2018 Nat. Mater. 17 432Google Scholar
[7] Yang M M, Luo Z D, Mi Z, Zhao J, Sharel P E, Alexe M 2020 Nature 584 377Google Scholar
[8] 郭少波, 闫世光, 曹菲, 姚春华, 王根水, 董显林 2020 物理学报 69 127708Google Scholar
Guo S B, Yan S G, Cao F, Yao C H, Wang G S, Dong X L 2020 Acta Phys. Sin. 69 127708Google Scholar
[9] Xu Y Q, Wu N J, Ignatiev A 2000 J. Appl. Phys. 88 1004Google Scholar
[10] Zhang S, Lebrun L, Jeong D Y, Randall C A, Zhang Q, Shrout T R 2003 J. Appl. Phys. 93 9257Google Scholar
[11] Huang X, Tang Y, Wang F, Ming Leung C, Zhao X, Qin X, Wang T, Duan Z, Wu Y, Wang J, Shi W 2022 J. Am. Ceram. Soc. 105 327Google Scholar
[12] He H, Lu X, Hanc E, Chen C, Zhang H, Lu L 2020 J. Mater. Chem. C 8 1494Google Scholar
[13] Song K, Ma N, Mishra Y K, Adelung R, Yang Y 2019 Adv. Electron. Mater. 5 1800413Google Scholar
[14] Srikanth K S, Singh V P, Vaish R 2017 J. Eur. Ceram. Soc. 37 3943Google Scholar
[15] Patel S, Weyland F, Tan X, Novak N 2018 Energy Technology 6 865Google Scholar
[16] Li L, Liu H, Wang R X, Zhang H, Huang H, Lu M H, Zhang S T, Jiang S, Wu D, Chen Y F 2020 J. Mater. Chem. C 8 7820Google Scholar
[17] Liu B, Li L, Zhang S T, Zhou L, Tan X 2022 J. Am. Ceram. Soc. 105 794Google Scholar
[18] Riemer L M, Lalitha K V, Jiang X, Liu N, Dietz C, Stark R W, Groszewicz P B, Buntkowsky G, Chen J, Zhang S T, Rodel J, Koruza J 2017 Act. Mater. 136 271Google Scholar
[19] Yin J, Wang Y, Zhang Y, Wu B, Wu J 2018 Act. Mater. 158 269Google Scholar
[20] Tabary P, Servant C, Alary J A 2000 J. Eur. Ceram. Soc. 20 913Google Scholar
[21] 田野, 靳立, 冯玉军, 庄永勇, 徐卓, 魏晓勇 2017 物理学进展 37 155
Tian Y, Jin L, Feng Y J, Zhuang Y Y, Xu Z, Wei X 2017 Prog. Phys. 37 155
[22] Wang H, Jiang B, Thomas R S, Cao W 2004 IEEE Trans. Ultrason. Ferr. 51 908Google Scholar
[23] Lee H J, Zhang S, Luo J, Li F, Shrout T R 2010 Adv. Funct. Mater. 20 3154Google Scholar
[24] Shen M, Hu Z, Qiu Y, Qiu S, Li M Y, Zhang G, Zhang S, Yang Z, Kagawa F, Jiang S 2019 J. Eur. Ceram. Soc. 39 5243Google Scholar
[25] You D, Tan H, Yan Z, Gao H, Chen S, Ma W, Fan P, Tran N M, Liu Y, Salamon D, Zhang H 2022 ACS Appl. Mater. Inter. 14 17652Google Scholar
[26] Tan X, Frederick J, Ma C, Aulbach E, Marsilius M, Hong W, Granzow T, Jo W, Rödel J 2010 Phys. Rev. B 81 014103Google Scholar
[27] Tan X, Jo W, Granzow T, Frederick J, Aulbach E, Rödel J 2009 Appl. Phys. Lett. 94 042909Google Scholar
[28] Frederick J, Tan X, Jo W 2011 J. Am. Ceram. Soc. 94 1149Google Scholar
[29] He H, Tan X 2007 J. Phys. Condens. Matter. 19 136003Google Scholar
[30] Tan X, Frederick J, Ma C, Jo W, Rodel J 2010 Phys. Rev. Lett. 105 255702Google Scholar
[31] Yang X, Zhuo F, Wang C, Liu Y, Wang Z, He C, Long X 2020 Act. Mater. 186 523Google Scholar
[32] Li S, Nie H, Wang G, Liu N, Zhou M, Cao F, Dong X 2019 J. Mater. Chem. C 7 4403Google Scholar
[33] Zhou M, Liang R, Zhou Z, Dong X 2019 J. Am. Ceram. Soc. 103 193Google Scholar
[34] Thakre A, Maurya D, Kim D Y, Kim Y, Sriboriboon P, Yoo I R, Priya S, Cho K H, Song H C, Ryu J 2021 J. Eur. Ceram. Soc. 41 2524Google Scholar
[35] Whatmore R W 2021 Encyclopedia Mater. Tech. Ceram. Glasses 3 139
[36] Qiao P, Zhang Y, Chen X, Zhou M, Wang G, Dong X 2019 Ceram. Int. 45 7114Google Scholar
[37] Jiang X P, Chen Y, Lam K H, Choy S H, Wang J 2010 J. Alloys Compd. 506 323Google Scholar
[38] Liu Z, Ren W, Peng P, Guo S, Lu T, Liu Y, Dong X, Wang G 2018 Appl. Phys. Lett. 112 142903Google Scholar
[39] Srikanth K S, Patel S, Steiner S, Vaish R 2018 Scr. Mater. 146 146Google Scholar
[40] Chen H, Guo S, Dong X, Cao F, Mao C, Wang G 2017 J. Alloys Compd. 695 2723Google Scholar
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图 2 (1–x)PNZST:xAlN (x = 0, 0.1, 0.2, 0.3和0.4)陶瓷的(a)—(e) SEM图像和(f)晶粒尺寸分布 (a) x = 0; (b) x = 0.1; (c) x = 0.2; (d) x = 0.3; (e) x = 0.4; (f)平均晶粒尺寸随AlN含量变化的关系
Fig. 2. The SEM images (a)–(e) and grain size distribution (f) of (1–x)PNZST:xAlN: (a) x = 0; (b) x = 0.1; (c) x = 0.2; (d) x = 0.3; (e) x = 0.4; (f) the composition dependence of average grain size.
图 6 不同组分(1–x)PNZST:xAlN陶瓷样品在室温不同电场下的P-E (a)—(e)和J-E (f)—(j)曲线 (a), (f) x = 0; (b), (g) x = 0.1; (c), (h) x = 0.2; (d), (i) x = 0.3; (e), (j) x = 0.4
Fig. 6. Electric field-dependent P-E loops (a)–(e) and J-E (f)–(j) curves of (1–x)PNZST:xAlN composite at room temperature: (a), (f) x = 0; (b), (g) x = 0.1; (c), (h) x = 0.2; (d), (i) x = 0.3; (e), (j) x = 0.4.
图 7 不同组分(1–x)PNZST:xAlN陶瓷样品在不同电场下的P-E (a)—(d)和J-E (e)—(h)曲线 (a), (e) x = 0.1; (b), (f) x = 0.2; (c), (g) x = 0.3; (d), (h) x = 0.4
Fig. 7. Temperature-dependent P-E loops (a)–(d) and J-E curves (e)–(h) of (1–x)PNZST:xAlN composite at room temperature: (a), (e) x = 0.1; (b), (f) x = 0.2; (c), (g) x = 0.3; (d), (h) x = 0.4.
表 1 PNZST:AlN复合陶瓷与其他已报道的无铅材料和PZT基材料的热释电性能参数比较
Table 1. Comparison of the pyroelectric parameters of PNZST:AlN ceramics, other reported lead-free materials and PZT-based materials.
材料组成 介电常数εr 介电损耗tanδ 热释电系数p/
(10–4 C·m–2·K–1)电流优值因子Fi/
(10–10 m·V–1)电压优值因子Fv/
(10–2 m2·C–1)探测率优值因子Fd/
(10–5 Pa–1/2)文献 TGS 55 0.025 5.5 2.12 43 6.1 [1] LiTaO3 crystal 47 0.0005 2.3 0.72 17 15.7 [1] PVDF 11 0.02 0.3 0.13 13.4 0.9 [35] BNT-BT 403 0.011 2.42 2.68 1.53 [2] BNT-BT-ST 1278 0.109 5.7 2.08 1.8 0.589 [2] PLZT 511 0.014 4.0 1.66 3.6 2.07 [36] KNN-BKT 980 0.035 2.18 0.994 1.14 0.57 [37] BNT-BA-KNN 514 0.029 3.7 1.32 2.89 1.15 [38] BCT-BST 3500 0.025 2.05 1 0.32 0.41 [39] CSBN 328 0.033 1.24 0.6 2.03 0.61 [40] PZT-based 290 0.0027 3.8 6.0 5.8 [2] KBT-BT-NBT 660 0.23 2.58 0.92 1.5 0.53 [34] PIMNT film 2824 0.004 8.5 3.40 1.4 1.03 [11] x = 0.1 583.6 0.01 33.0 31.6 61.3 44.0 本工作 -
[1] Liu Z, Lu T, Dong X, Wang G, Liu Y 2021 IEEE Trans. Ultrason. Ferr. 68 242Google Scholar
[2] Jia J, Guo S, Yan S, Cao F, Yao C, Dong X, Wang G 2019 Appl. Phys. Lett. 114 032902Google Scholar
[3] Whatmore R W 1986 Rep. Prog. Phys. 49 1135Google Scholar
[4] Wang Y, Yuan G, Luo H, Li J, Viehland D 2017 Phys. Rev. Appl. 8 034032Google Scholar
[5] Domingo N, Bagués N, Santiso J, Catalan G 2015 Phys. Rev. B 91 094111Google Scholar
[6] Pandya S, Wilbur J, Kim J, Gao R, Dasgupta A, Dames C, Martin L W 2018 Nat. Mater. 17 432Google Scholar
[7] Yang M M, Luo Z D, Mi Z, Zhao J, Sharel P E, Alexe M 2020 Nature 584 377Google Scholar
[8] 郭少波, 闫世光, 曹菲, 姚春华, 王根水, 董显林 2020 物理学报 69 127708Google Scholar
Guo S B, Yan S G, Cao F, Yao C H, Wang G S, Dong X L 2020 Acta Phys. Sin. 69 127708Google Scholar
[9] Xu Y Q, Wu N J, Ignatiev A 2000 J. Appl. Phys. 88 1004Google Scholar
[10] Zhang S, Lebrun L, Jeong D Y, Randall C A, Zhang Q, Shrout T R 2003 J. Appl. Phys. 93 9257Google Scholar
[11] Huang X, Tang Y, Wang F, Ming Leung C, Zhao X, Qin X, Wang T, Duan Z, Wu Y, Wang J, Shi W 2022 J. Am. Ceram. Soc. 105 327Google Scholar
[12] He H, Lu X, Hanc E, Chen C, Zhang H, Lu L 2020 J. Mater. Chem. C 8 1494Google Scholar
[13] Song K, Ma N, Mishra Y K, Adelung R, Yang Y 2019 Adv. Electron. Mater. 5 1800413Google Scholar
[14] Srikanth K S, Singh V P, Vaish R 2017 J. Eur. Ceram. Soc. 37 3943Google Scholar
[15] Patel S, Weyland F, Tan X, Novak N 2018 Energy Technology 6 865Google Scholar
[16] Li L, Liu H, Wang R X, Zhang H, Huang H, Lu M H, Zhang S T, Jiang S, Wu D, Chen Y F 2020 J. Mater. Chem. C 8 7820Google Scholar
[17] Liu B, Li L, Zhang S T, Zhou L, Tan X 2022 J. Am. Ceram. Soc. 105 794Google Scholar
[18] Riemer L M, Lalitha K V, Jiang X, Liu N, Dietz C, Stark R W, Groszewicz P B, Buntkowsky G, Chen J, Zhang S T, Rodel J, Koruza J 2017 Act. Mater. 136 271Google Scholar
[19] Yin J, Wang Y, Zhang Y, Wu B, Wu J 2018 Act. Mater. 158 269Google Scholar
[20] Tabary P, Servant C, Alary J A 2000 J. Eur. Ceram. Soc. 20 913Google Scholar
[21] 田野, 靳立, 冯玉军, 庄永勇, 徐卓, 魏晓勇 2017 物理学进展 37 155
Tian Y, Jin L, Feng Y J, Zhuang Y Y, Xu Z, Wei X 2017 Prog. Phys. 37 155
[22] Wang H, Jiang B, Thomas R S, Cao W 2004 IEEE Trans. Ultrason. Ferr. 51 908Google Scholar
[23] Lee H J, Zhang S, Luo J, Li F, Shrout T R 2010 Adv. Funct. Mater. 20 3154Google Scholar
[24] Shen M, Hu Z, Qiu Y, Qiu S, Li M Y, Zhang G, Zhang S, Yang Z, Kagawa F, Jiang S 2019 J. Eur. Ceram. Soc. 39 5243Google Scholar
[25] You D, Tan H, Yan Z, Gao H, Chen S, Ma W, Fan P, Tran N M, Liu Y, Salamon D, Zhang H 2022 ACS Appl. Mater. Inter. 14 17652Google Scholar
[26] Tan X, Frederick J, Ma C, Aulbach E, Marsilius M, Hong W, Granzow T, Jo W, Rödel J 2010 Phys. Rev. B 81 014103Google Scholar
[27] Tan X, Jo W, Granzow T, Frederick J, Aulbach E, Rödel J 2009 Appl. Phys. Lett. 94 042909Google Scholar
[28] Frederick J, Tan X, Jo W 2011 J. Am. Ceram. Soc. 94 1149Google Scholar
[29] He H, Tan X 2007 J. Phys. Condens. Matter. 19 136003Google Scholar
[30] Tan X, Frederick J, Ma C, Jo W, Rodel J 2010 Phys. Rev. Lett. 105 255702Google Scholar
[31] Yang X, Zhuo F, Wang C, Liu Y, Wang Z, He C, Long X 2020 Act. Mater. 186 523Google Scholar
[32] Li S, Nie H, Wang G, Liu N, Zhou M, Cao F, Dong X 2019 J. Mater. Chem. C 7 4403Google Scholar
[33] Zhou M, Liang R, Zhou Z, Dong X 2019 J. Am. Ceram. Soc. 103 193Google Scholar
[34] Thakre A, Maurya D, Kim D Y, Kim Y, Sriboriboon P, Yoo I R, Priya S, Cho K H, Song H C, Ryu J 2021 J. Eur. Ceram. Soc. 41 2524Google Scholar
[35] Whatmore R W 2021 Encyclopedia Mater. Tech. Ceram. Glasses 3 139
[36] Qiao P, Zhang Y, Chen X, Zhou M, Wang G, Dong X 2019 Ceram. Int. 45 7114Google Scholar
[37] Jiang X P, Chen Y, Lam K H, Choy S H, Wang J 2010 J. Alloys Compd. 506 323Google Scholar
[38] Liu Z, Ren W, Peng P, Guo S, Lu T, Liu Y, Dong X, Wang G 2018 Appl. Phys. Lett. 112 142903Google Scholar
[39] Srikanth K S, Patel S, Steiner S, Vaish R 2018 Scr. Mater. 146 146Google Scholar
[40] Chen H, Guo S, Dong X, Cao F, Mao C, Wang G 2017 J. Alloys Compd. 695 2723Google Scholar
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