具有本征低晶格热导率的硫化银快离子导体的热电性能

王拓; 陈弘毅; 仇鹏飞; 史迅; 陈立东

doi:10.7498/aps.68.20190073

摘要

硫化银(Ag₂S)是一种典型的快离子导体材料, 前期关于Ag₂S的研究主要集中在光电和生物等领域. 最近的研究表明, α-Ag₂S具有和金属一样的良好延展性和变形能力. 但是, Ag₂S的热电性能尚无公开报道. 本工作合成了单相Ag₂S化合物, 系统研究了其在300—600 K范围的物相变化、离子迁移特性和电热输运性质. 研究发现, Ag₂S在300—600 K温度区间表现出半导体的电输运性质. 由于单斜-体心立方相晶体结构转变, Ag₂S的离子电导率、载流子浓度、迁移率、电导率、泽贝克系数等性质在455 K前后出现急剧变化. 在550 K, Ag₂S的功率因子最高可达5 μW·cm^–1·K^–2. Ag₂S在300—600 K温度区间均表现出本征的低晶格热导率(低于0.6 W·m^–1·K^–1). S亚晶格中随机分布的类液态Ag离子是导致β-Ag₂S体心立方相具有低晶格热导率的主要原因. 在573 K, Ag₂S的热电优值可达0.55, 与Ag₂Se, Ag₂Te, CuAgSe等已报道的Ag基快离子导体热电材料的性能相当.

关键词:

Abstract

Recently, Ag₂S superionic conductor has attracted great attention due to its metal-like ductility and deformability. In this work, the single phase Ag₂S compound is fabricated by the melting-annealing method. The crystal structure, ionic conduction, and electrical and thermal transports in a temperature range of 300－600 K are systematically investigated. The monoclinic-cubic crystal structure transition occurs around 455 K for Ag₂S. Significant reduction in the specific heat at constant volume below the Dulong-Petit limit is observed for Ag₂S after the monoclinic-cubic phase transition, which is attributed to the liquid-like Ag ions existing inside the sulfur framework. Ag₂S shows typical semiconducting-like electrical transport behavior in the whole measured temperature range. Around 455 K, the ionic conductivity, carrier concentration, carrier mobility, electrical conductivity, and Seebeck coefficient each show an abrupt change. The calculated ionic activation based on the ionic conductivity is 0.076 eV for the body centered cubic Ag₂S. The calculated band gap based on the electrical conductivity decreases from 1.1 eV for the monoclinic Ag₂S to 0.42 eV for the body centered cubic Ag₂S. The abrupt increase of electrical conductivity after the monoclinic-cubic phase transition leads to a maximum power factor around 5 μW·cm^–1·K^–2 at 550 K. In the whole measured temperature range, Ag₂S demonstrates an intrinsically low lattice thermal conductivity (below 0.6 W·m^–1·K^–1). The calculated phonon dispersion indicates that the weak chemical bonding between Ag and S is responsible for the low lattice thermal conductivity observed in the monoclinic Ag₂S. Likewise, the presence of liquid-like Ag ions with low ionic activation energy is responsible for the low lattice thermal conductivity for the cubic Ag₂S. Finally, the Ag₂S shows the maximum thermoelectric figure of merit of 0.55 at 580 K, which is comparable to the thermoelectric figure of merit reported before in most of Ag-based thermoelectric superionic conductors.

Keywords:

作者及机构信息

1.
中国科学院上海硅酸盐研究所, 高性能陶瓷和超微结构国家重点实验室, 上海　200050

2.
中国科学院大学, 材料与光电研究中心, 北京　100049

3.
上海交通大学, 材料科学与工程学院, 上海　200240

通信作者: 仇鹏飞, qiupf@mail.sic.ac.cn ; 史迅, xshi@mail.sic.ac.cn ;

基金项目: 国家重点研发计划(批准号: 2018YFB0703600)、国家自然科学基金杰出青年科学基金(批准号: 51625205)、中国科学院重点部署项目(批准号: KFZD-SW-421)和中国科学院青年创新促进会(批准号：2016232)资助的课题.

Authors and contacts

1.
State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China

2.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

3.
School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China

Corresponding author: Qiu Peng-Fei, qiupf@mail.sic.ac.cn ; Shi Xun, xshi@mail.sic.ac.cn ;

Funds: Project supported by the National Key Research and Development Program of China (Grant No. 2018YFB0703600), the National Natural Science Foundation of China (Grant No. 51625205), the Key Research Program of Chinese Academy of Sciences (Grant No. KFZD-SW-421), and the Youth Innovation Promotion Association, CAS (Grant No. 2016232).

文章全文 : translate this paragraph

参考文献

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施引文献

图 1 Ag₂S化合物在(a) 300 K和(b) 600 K时的块体XRD图谱

Fig. 1. Bulk XRD patterns of Ag₂S compound at (a) 300 K and (b) 600 K.

下载: 全尺寸图片幻灯片

图 2 Ag₂S化合物的(a)背散射电子图片; (b)所有元素, (c) Ag和(d) S的元素分布

Fig. 2. (a) Backscattering image of Ag₂S compound. Elemental mappings of (b) all elements, (c) Ag, and (d) S, respectively.

下载: 全尺寸图片幻灯片

图 3 Ag₂S化合物的(a)定压热容C_p及(b)相同温度下的C_p和定容热容C_V计算值的比较, 其中点划线分别为固体的C_V理论值3Nk_B和液体的C_V理论值2Nk_B

Fig. 3. (a) Specific heat at constant pressure C_p of Ag₂S compound; (b) comparison of C_p and the calculated specific heat at constant volume C_V. The dash-dot lines are the theoretical C_V of solid and liquid, respectively.

下载: 全尺寸图片幻灯片

图 4 Ag₂S化合物的离子电导率(σ_i)随温度的变化

Fig. 4. Temperature dependence of ionic conductivity (σ_i) for Ag₂S compound.

下载: 全尺寸图片幻灯片

图 5 Ag₂S化合物的(a)载流子浓度n_H和(b)载流子迁移率$ {{\mu} _{\rm{H}}}$随温度的变化

Fig. 5. Temperature dependences of (a) carrier concentration n_H and (b) carrier mobility $ {{\mu} _{\rm{H}}}$ for Ag₂S compound.

下载: 全尺寸图片幻灯片

图 6 Ag₂S化合物的(a)泽贝克系数S、(b)电导率σ、(c)功率因子PF随温度的变化

Fig. 6. Temperature dependences of (a) Seebeck coefficient S, (b) electrical conductivity σ, and (c) power factor (PF) for Ag₂S compound.

下载: 全尺寸图片幻灯片

图 7 Ag₂S化合物的(a)总热导率κ和(b)晶格热导率κ_L随温度的变化, 图(b)中虚线所示为Cu₂Se^[5]和Cu₂S^[37]快离子导体热电材料的晶格热导率

Fig. 7. Temperature dependences of (a) total thermal concentration κ and (b) lattice thermal conductivity κ_L for Ag₂S compound. The κ_L data for Cu₂Se^[5] and Cu₂S^[37] are included for comparison in panel (b).

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图 8 Ag₂S的声子色散关系和声子态密度图

Fig. 8. Phonon dispersion relations and density of states for Ag₂S compound.

下载: 全尺寸图片幻灯片

图 9 Ag₂S化合物的热电优值zT随温度的变化, 虚线所示为Ag₂Se^[30], Ag₂Te^[31]和CuAgSe^[10]等Ag基快离子导体热电材料的热电优值

Fig. 9. Temperature dependence of thermoelectric figure-of-merit zT for Ag₂S compound. The data for Ag₂Se^[30], Ag₂Te^[31] and CuAgSe^[10] are included for comparison.

下载: 全尺寸图片幻灯片

[1]	Tan G, Zhao L, Kanatzidis M G 2016 Chem. Rev. 116 12123 Google Scholar
[2]	Zeier W G, Zevalkink A, Gibbs Z M, Hautier G, Kanatzidis M G, Snyder G J 2016 Angew. Chem: Int. Ed. 55 6826 Google Scholar
[3]	Shi X, Chen L, Uher C 2016 Int. Mater. Rev. 61 379 Google Scholar
[4]	Zhu T, Liu Y, Fu C, Heremans J P, Snyder J G, Zhao X 2017 Adv. Mater. 29 1605884 Google Scholar
[5]	Liu H, Shi X, Xu F, Zhang L, Zhang W, Chen L, Li Q, Uher C, Day T, Snyder J G 2012 Nat. Mater. 11 422 Google Scholar
[6]	Zhao K, Qiu P, Song Q, Blichfeld A B, Eikeland E, Ren D, Ge B, Iversen B B, Shi X, Chen L 2017 Mater. Today Phys. 1 14 Google Scholar
[7]	Zhu C, He Y, Lu P, Fu Z, Xu F, Yao H, Zhang L, Shi X, Chen L 2017 Ceram. Int. 43 7866 Google Scholar
[8]	Zhao K, Guan M, Qiu P, Blichfeld A B, Eikeland E, Zhu C, Ren D, Xu F, Iversen B B, Shi X, Chen L 2018 J. Mater. Chem. A 6 6977 Google Scholar
[9]	Lü Y, Chen J, Max D, Li Y, Shi X, Chen L 2015 J. Inorg. Mater. 30 1115 Google Scholar
[10]	Wang X, Qiu P, Zhang T, Ren D, Wu L, Shi X, Yang J, Chen L 2015 J. Mater. Chem. A 3 13662 Google Scholar
[11]	Bhattacharya S, Basu R, Bhatt R, Pitale S, Singh A, Aswal D K, Gupta S K, Navaneethan M, Hayakawa Y 2013 J. Mater. Chem. A 1 11289 Google Scholar
[12]	Jiang B, Qiu P, EikelandE, Chen H, Song Q, Ren D, Zhang T, Yang J, Iversen B B, Shi X, Chen L 2017 J. Mater. Chem. C 5 943 Google Scholar
[13]	Jiang B, Qiu P, Chen H, Zhang Q, Zhao K, Ren D, Shi X, Chen L 2017 Chem. Commun. 53 11658 Google Scholar
[14]	Shi X, Chen H, Hao F, Liu R, Wang T, Qiu P, Burkhardt U, Grin Y, Chen L 2018 Nat. Mater. 17 421 Google Scholar
[15]	Rahlfs P 1936 Zeitschrift für Phys. Chem. 31B 157
[16]	Skinner B J 1966 Econ. Geol. 61 1 Google Scholar
[17]	董占民, 孙红三, 许佳, 李一, 孙家林 2011 物理学报 60 077304 Google Scholar Dong Z M, Sun H S, Xu J, Li Y, Sun J L 2011 Acta Phys. Sin. 60 077304 Google Scholar
[18]	Yang J, Ying J Y 2011 Angew. Chem.: Int. Ed. 50 4637 Google Scholar
[19]	Khanchandani S, Srivastava P K, Kumar S, Ghosh S, Ganguli A K 2014 Inorg. Chem. 53 8902 Google Scholar
[20]	ZhangY, Hong G, ZhangY, Chen G, Li F, Dai H, Wang Q 2012 ACS Nano 6 3695 Google Scholar
[21]	Du Y, Xu B, Fu T, Cai M, Li F, Zhang Y, Wang Q 2010 J. Am. Chem. Soc. 132 1470 Google Scholar
[22]	邓立儿, 李妍, 巩蕾, 王佳 2018 无机材料学报 33 825 Deng L, Li Y, Gong L, Wang J 2018 J. Inorg. Mater. 33 825
[23]	Hong G, Robinson J T, Zhang Y, Diao S, Antaris A L, Wang Q, Dai H 2012 Angew. Chem.: Int. Ed. 51 9818 Google Scholar
[24]	Pei Y, Shi X, Lalonde A, Wang H, Chen L, Snyder G J 2011 Nature 473 66 Google Scholar
[25]	张玉, 吴立华, 曾李骄开, 刘叶烽, 张继业, 王佳, 邢娟娟, 骆军 2016 物理学报 65 107201 Google Scholar Zhang Y, Wu L H, Zeng L J K, Liu Y F, Zhang J Y, Wang J, Xing J J, Luo J 2016 Acta Phys. Sin. 65 107201 Google Scholar
[26]	杨小燕, 吴洁华, 任都迪, 张天松, 陈立东 2016 无机材料学报 31 997 Yang X Y, Wu J H, Ren D D, Zhang T S, Chen L D 2016 J. Inorg. Mater. 31 997
[27]	Biswas K, He J, Blum I D, Wu C I, Hogan T P, Seidman D N, Dravid V P, Kanatzidis M G 2012 Nature 489 414 Google Scholar
[28]	Shi X, Zhang W, Chen L, Yang J 2005 Phys. Rev. Lett. 95 185503 Google Scholar
[29]	姚铮, 仇鹏飞, 李小亚, 陈立东 2016 无机材料学报 31 1375 Yao Z, Qiu P F, Li X Y, Chen L D 2016 J. Inorg. Mater. 31 1375
[30]	Day T, Drymiotis F, Zhang T, Rhodes D, Shi X, Chen L, Snyder G J 2013 J. Mater. Chem. C 1 7568 Google Scholar
[31]	Pei Y, Heinz N A, Snyder G J 2011 J. Mater. Chem. 21 18256 Google Scholar
[32]	Liu Y, Qiu P, Chen H, Chen R, Shi X, Chen L 2017 J. Inorg. Mater. 32 1337 Google Scholar
[33]	Tsuchiya Y, Tamaki S, Waseda Y, Toguri J M 1978 J. Phys. C: Solid State Phys. 11 651 Google Scholar
[34]	Blanton T, Misture S, Dontula N, Zdzieszynski S 2011 Powder Diffr. 26 114 Google Scholar
[35]	Honma K, Iida K 1987 J. Phys. Soc. Japan 56 1828 Google Scholar
[36]	Ishiwata S, Shiomi Y, Lee J S, Bahramy M S, Suzuki T, Uchida M, Arita R, Taguchi Y, Tokura Y 2013 Nat. Mater. 12 512 Google Scholar
[37]	He Y, Da yT, Zhang T, Liu H, Shi X, Chen L, Snyder G J 2014 Adv. Mater. 26 3974 Google Scholar
[38]	Liu H, YuanX, Lu P, Shi X, Xu F, He Y, Tang Y, Bai S, Zhang W, Chen L, Lin Y, Shi L, Lin H, Gao X, Zhang X, Chi H, Uher C 2013 Adv. Mater. 25 6607 Google Scholar
[39]	Aliev F F, Jafarov M B, Tairov B A, Pashaev G P, Saddinova A A, Kuliev A A 2008 Semiconductors 42 1146 Google Scholar
[40]	Balapanov M K, Gafurov I G, Mukhamed'yanov U K, Yakshibaev R A, Ishembetov R K 2004 Phys. Status Solidi B 241 114 Google Scholar
[41]	Mi W, Qiu P, Zhang T, Lü Y, Shi X, Chen L 2014 Appl. Phys. Lett. 104 133903 Google Scholar
[42]	Xiao C, Xu J, Li K, Feng J, Yang J, Xie Y 2012 J. Am. Chem. Soc. 134 4287 Google Scholar
[43]	He Y, Lu P, Shi X, Xu F, Zhang T, Snyder G J, Uher C, Chen L 2015 Adv. Mater. 27 3639 Google Scholar
[44]	Qiu P, Qin Y, Zhang Q, Li R, Yang J, Song Q, Tang Y, Bai S, Shi X, Chen L 2018 Adv. Sci. 5 1700727 Google Scholar

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具有本征低晶格热导率的硫化银快离子导体的热电性能