Sm3+掺杂0.94Bi0.5Na0.5TiO3-0.06BaTiO3无机多功能陶瓷的储能行为和光致发光性质

郑明; 杨健; 张怡笑; 关朋飞; 程奥; 范贺良

doi:10.7498/aps.72.20230685

摘要

近年来, 无机多功能材料在各个领域得到了广泛的应用. 掺杂稀土的铁电材料作为一种新型的无机多功能材料具有很大的潜力. 本文系统地研究了Sm³⁺掺杂的0.94Bi_0.5Na_0.5TiO₃-0.06BaTiO₃(BNTBT)陶瓷的铁电、储能行为和光致发光性能. 结果表明, Sm³⁺的引入有效地抑制了BNTBT的晶粒生长, 导致剩余极化(P_r)和矫顽场(E_c)明显下降. 在60 kV/cm的外加电场下, 当Sm³⁺掺杂浓度为0.6%时, W_rec达到最大值0.27 J/cm³. 储能效率(η)随着电场的增加而逐渐降低, 在掺杂浓度大于0.6%时稳定在45%附近. 此外, 在408 nm的近紫外光的激发下, 所有Sm³⁺掺杂的样品都表现出可见光的输出, 当Sm³⁺的掺杂量为1.0%时发光强度达到最大, 在701 nm处(⁴G_5/2→⁶H_11/2)发光强度的相对变化(ΔI/I)达到700%. 本文制备了一种同时具有储能和光致发光特性的新型陶瓷, 为无机多功能材料的开发提供了一种有希望的策略.

关键词:

稀土 /
铁电 /
储能 /
光致发光

Abstract

In recent years, inorganic multifunctional ferroelectric ceramics have been widely utilized in various fields, including aerospace, optical communication, and capacitors, owing to their high stability, easy synthesis, and flexibility. Rare-earth doped ferroelectric materials hold immense potential as a new type of inorganic multifunctional material. This work focuses on the synthesis of x%Sm³⁺-doped 0.94Bi_0.5Na_0.5TiO₃-0.06BaTiO₃ (BNTBT:x%Sm³⁺ in short) ceramics by using the conventional solid-state sintering method, aiming to comprehensively investigate their ferroelectric, energy storage, and photoluminescence (PL) properties. The X-ray diffraction analysis reveals that the introduction of Sm³⁺ does not trigger off the appearing of secondary phases or changing of the original perovskite structure. The scanning electron microscope (SEM) images demonstrate that Sm³⁺ incorporation effectively restrains the grain growth in BNTBT, resulting in the average grain size decreasing from 1.16 to 0.95 μm. The reduction in remanent polarization (P_r) and coercive field (E_c) can be attributed to both the grain size refinement and the formation of morphotropic phase boundaries (MPBs). Under an applied field of 60 kV/cm, the maximum value of energy storage density (W_rec) reaches to 0.27 J/cm³ at an Sm³⁺ doping concentration of 0.6%. The energy storage efficiency (η) gradually declines with electric field increasing and stabilizes at approximately 45% for Sm³⁺ doping concentrations exceeding 0.6%. This result can be ascribed to the decrease in ΔP (P_max– P_r) due to the growth of ferroelectric domains as the electric field increases. Additionally, all Sm³⁺-doped BNTBT ceramics exhibit outstanding PL performance upon being excited with near-ultraviolet (NUV) light at 408 nm, without peak position shifting. The PL intensity peaks when the Sm³⁺ doping concentration is 1.0%, with a relative change (ΔI/I) reaching to 700% at 701 nm (⁴G_5/2→⁶H_11/2). However, the relative change in PL intensity is minimum at 562 nm (⁴G_5/2→⁶H_5/2) due to the fact that the ⁴G_5/2→⁶H_5/2 transition represents a magnetic dipole transition, and the PL intensity remains relatively stable despite variations in the crystal field environment surrounding Sm³⁺. Our successful synthesis of this novel ceramic material, endowed with both energy storage and PL properties, offers a promising avenue for developing inorganic multifunctional materials. The Sm³⁺-doped BNTBT ceramics hold considerable potential applications in optical memory and multifunctional capacitors.

Keywords:

作者及机构信息

中国矿业大学材料与物理学院, 徐州　221116

通信作者: 郑明, zhengm@mail.ustc.edu.cn

基金项目: 中央高校基本科研业务费专项资金(批准号: 2022QN1087)资助的课题.

Authors and contacts

School of Materials Science and Physics, China University of Mining and Technology, Xuzhou 221116, China

Corresponding author: Zheng Ming, zhengm@mail.ustc.edu.cn

Funds: Project supported by the Fundamental Research Funds for the Central Universities, China (Grant No. 2022QN1087).

文章全文 : translate this paragraph

参考文献

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施引文献

图 1 XRD θ-2θ扫描图谱

Fig. 1. XRD θ-2θ scan pattern.

下载: 全尺寸图片幻灯片

图 2 (a)—(f) BNTBT:x%Sm³⁺(x = 0, 0.2, 0.4, 0.6, 0.8, 1.0)的SEM照片和晶粒尺寸分布图

Fig. 2. (a)–(f) SEM images and grain size distribution patterns of BNTBT: x%Sm³⁺ (x = 0, 0.2, 0.4, 0.6, 0.8, 1.0).

下载: 全尺寸图片幻灯片

图 3 BNTBT:x%Sm³⁺　(a) 电滞回线; (b) P_r和E_c随掺杂浓度的变化图

Fig. 3. BNTBT:x%Sm³⁺: (a) P-E loops; (b) the image of the variation of P_r and E_c.

下载: 全尺寸图片幻灯片

图 4 BNTBT:x%Sm³⁺ (a) 单极P-E曲线, (b) W_rec, (c) η, (d) W_rec和η在60 kV/cm随掺杂浓度的变化

Fig. 4. (a) Single P-E loops, (b) W_rec, (c) η, and (d) W_rec and η changes at 60 kV/cm under diverse doping concentrations for BNTBT:x%Sm³⁺samples.

下载: 全尺寸图片幻灯片

图 5 (a) BNTBT:0.2%Sm³⁺陶瓷PL激发光谱; (b) 不同掺杂浓度在408 nm光激发下的发射光谱; (c) 不同发射峰的PL强度变化图; (d) ΔI/I图

Fig. 5. (a) PLE spectrum of BNTBT:0.2%Sm³⁺ ceramic; (b) PL spectrum under 408 nm excitation with diverse doping concentrations; (c) the PL intensity change diagram at different emission peaks; (d) the diagram of ΔI/I.

下载: 全尺寸图片幻灯片

[1]	Famprikis T, Canepa P, Dawson J A, Islam M S, Masquelier C 2019 Nat. Mater. 18 1278 Google Scholar
[2]	Guo P F, Su L, Peng K, Lu D, Xu L, Li M Z, Wang H J 2022 ACS Nano 16 6625 Google Scholar
[3]	Zheng B Z, Fan J Y, Chen B, Qin X, Wang J, Wang F, Deng R R, Liu X G 2022 Chem. Rev. 122 5519 Google Scholar
[4]	Nazir H, Batool M, Osorio F J B, Isaza-Ruiz M, Xu X H, Vignarooban K, Phelan P, Inamuddin, Kannan A M 2019 Int. J. Heat Mass Transfer 129 491 Google Scholar
[5]	Wen Q B, Qu F M, Yu Z J, Graczyk Zajac M, Xiong X, Riedel R 2022 J. Adv. Ceram. 11 197 Google Scholar
[6]	Yu R, Zhang H L, Guo B L 2022 Nano-Micro Lett. 14 1 Google Scholar
[7]	Zheng X T, Ananthanarayanan A, Luo K Q, Chen P 2015 Small 11 1620 Google Scholar
[8]	Zhang X Q, Zhang K Q, Zhang B, Li Y, He R J 2022 J. Adv. Ceram. 11 1918 Google Scholar
[9]	包定华 2020 物理学报 69 127712 Google Scholar Bao D H 2020 Acta Phys. Sin. 69 127712 Google Scholar
[10]	Zhu D Y, Nikl M, Chewpraditkul W, Li J 2022 J. Adv. Ceram. 11 1825 Google Scholar
[11]	Zou H, Yu Y, Li J, Cao Q F, Wang X S, Hou J W 2015 Mater. Res. Bull. 69 112 Google Scholar
[12]	Hao S L, Li J H, Sung Q B, Wei L L, Yang Z P 2019 J. Mater. Sci. -Mater. Electron. 30 13372 Google Scholar
[13]	Hao S L, Li J H, Yang P, Wei L L, Yang Z P 2017 J. Am. Ceram. Soc. 100 5620 Google Scholar
[14]	He J Y, Zhang J J, Xing H J, Pan H L, Jia X R, Wang J Y, Zheng P 2017 Ceram. Int. 43 250 Google Scholar
[15]	Jia Q, Zhang Q, Sun H, Hao X 2021 J. Eur. Ceram. Soc. 41 1211 Google Scholar
[16]	Jia Q N, Li Y, Guan L L, Sun H Q, Zhang Q W, Hao X H 2020 J. Mater. Sci. -Mater. Electron. 31 19277 Google Scholar
[17]	Hui X W, Peng D F, Zou H, Li J, Cao Q F, Li Y X, Wang X S, Yao X 2014 Ceram. Int. 40 12477 Google Scholar
[18]	Li W, Wang Z, Hao J G, Fu P, Du J, Chu R Q, Xu Z J 2018 J. Mater. Chem. C 6 11312 Google Scholar
[19]	Liu Y, Luo H, Zhai D, Zeng L, Xiao Z, Hu Z, Wang X, Zhang D 2022 ACS Appl. Mater. Interfaces 14 19376 Google Scholar
[20]	Qin Y L, Zhang S J, Wu Y Q, Lu C J, Zhang J L 2017 J. Eur. Ceram. Soc. 37 3493 Google Scholar
[21]	Yang Z T, Du H L, Jin L, Poelman D 2021 J. Mater. Chem. A 9 18026 Google Scholar
[22]	Cao R P, Wang W H, Ren Y, Hu Z F, Zhou X C, Xu Y C, Luo Z Y, Liang A H 2021 J. Lumin. 235 118054 Google Scholar
[23]	Sun H Q, Liu J, Wang X S, Zhang Q W, Hao X H, An S L 2017 J. Mater. Chem. C 5 9080 Google Scholar
[24]	Lü J W, Li Q, Li Y, Tang M Y, Jin D L, Yan Y, Fan B Y, Jin L, Liu G 2021 Chem. Eng. J. 420 129900 Google Scholar
[25]	Du P, Yu J S 2015 Ceram. Int. 41 6710 Google Scholar
[26]	Said S, Marchet P, Merle Mejean T, Mercurio J P 2004 Mater. Lett. 58 1405 Google Scholar
[27]	Choi H, Cho S H, Khan S, Lee K R, Kim S 2014 J. Mater. Chem. C 2 6017 Google Scholar
[28]	Lun M M, Wang W, Xing Z F, Wan Z, Wu W Y, Song H Z, Wang Y Z, Li W, Chu B L, He Q Y 2019 J. Am. Ceram. Soc. 102 5243 Google Scholar
[29]	Xue J P, Noh H M, Choi B C, Park S H, Kim J H, Jeong J H, Du P 2020 Chem. Eng. J. 382 122861 Google Scholar
[30]	Li F F, Liu Y F, Lyu Y N, Qi Y H, Yu Z L, Lu C G 2017 Ceram. Int. 43 106 Google Scholar
[31]	Han K, Luo N N, Chen Z P, Ma L, Chen X Y, Feng Q, Hu C Z, Zhou H F, Wei Y Z, Toyohisa F 2020 J. Eur. Ceram. Soc. 40 3562 Google Scholar
[32]	Zhang M H, Qi J L, Liu Y Q, Lan S, Luo Z X, Pan H, Lin Y H 2022 Rare Metals 41 730 Google Scholar
[33]	Huang Y, Zhao C, Wu B, Zhang X 2022 J. Eur. Ceram. Soc. 42 2764 Google Scholar
[34]	Muthuramalingam M, Ruth D E J, Babu M V G, Ponpandian N, Mangalaraj D, Sundarakannan B 2016 Scr. Mater. 112 58 Google Scholar
[35]	Zheng M, Guan P, Ji X 2023 CrystEngComm 25 541 Google Scholar
[36]	Guan P F, Zhang Y X, Yang J, Zheng M 2023 Ceram. Int. 49 11796 Google Scholar
[37]	Ma C L, Wang X Y, Tan W S, Zhou W P, Wang X X, Cheng Z Z, Chen G B, Zhai Z Y 2020 Dalton Trans. 49 5581 Google Scholar
[38]	Yang Z T, Du H L, Qu S B, Hou Y D, Ma H, Wang J F, Wang J, Wei X Y, Xu Z 2016 J. Mater. Chem. A 4 13778 Google Scholar
[39]	Zhang Y M, Liang G C, Tang S L, Peng B L, Zhang Q, Liu L J, Sun W H 2020 Ceram. Int. 46 1343 Google Scholar
[40]	杜金华, 李雍, 孙宁宁, 赵烨, 郝喜红 2020 物理学报 69 127703 Google Scholar Du J H, Li Y, Sun N N, Zhao Y, Hao X H 2020 Acta Phys. Sin. 69 127703 Google Scholar
[41]	Wei T, Sun F C, Zhao C Z, Li C P, Yang M, Wang Y Q 2013 Ceram. Int. 39 9823 Google Scholar
[42]	Singh V, Watanabe S, Rao T K G, Chubaci J F D, Kwak H Y 2010 J. Non-Cryst. Solids 356 1185 Google Scholar
[43]	Raju G S R, Pavitra E, Patnam H, Varaprasad G L, Chodankar N R, Patil S J, Ranjith K S, Rao M V B, Yu J S, Park J Y, Huh Y S, Han Y K 2022 J. Alloys Compd. 903 163881 Google Scholar

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Sm³⁺掺杂0.94Bi_0.5Na_0.5TiO₃-0.06BaTiO₃无机多功能陶瓷的储能行为和光致发光性质