Cu1.8–x Sbx S热电材料的相结构与电热输运性能

赵英浩; 张瑞; 张波萍; 尹阳; 王明军; 梁豆豆

doi:10.7498/aps.70.20201852

摘要

Cu_1.8S基热电材料因其丰富的原料储备、低毒性及优良的电学和热学性能而成为具有应用潜力的热电材料. 本文采用机械合金化(mechanical alloying, MA)结合放电等离子烧结(spark plasma sintering, SPS)工艺制备了一系列Cu_1.8–x Sb_x S (x = 0, 0.005, 0.02, 0.03, 0.04)块体材料, 研究了不同Sb掺杂量对Cu_1.8–x Sb_x S相结构、微观形貌及热电性能的影响. 结果表明, 随着Sb含量的增加, Cu_1.8–x Sb_x S材料相结构由单相Cu_1.8S转变为多相共存, 其块体均呈p型导电特征. 样品Cu_1.77Sb_0.03S在723 K时取得最高ZT值约为0.37, 比未掺杂Cu_1.8S(0.33)提高了12%.

关键词:

Abstract

Cu_1.8S-based materials have become potential thermoelectric materials due to their rich raw material reserves, low toxicity, and excellent electrical and thermal properties. In this study, a series of Cu_1.8–x Sb_x S (x = 0, 0.005, 0.02, 0.03, 0.04) bulk materials is synthesized by using mechanical alloying combined with spark plasma sintering process. This preparation method can shorten the preparation cycle of materials, and effectively improve the research and development efficiency of thermoelectric (TE) materials due to its simple process. The effects of different Sb doping amounts on the structure, micromorphology, and thermoelectric transport properties of Cu_1.8–x Sb_x S phase are investigated. The results show that when 0 ≤ x < 0.02, the bulk samples are single-phase Cu_1.8S. With the further increase of Sb doping to 0.02 ≤ x ≤ 0.04, the second phase CuSbS₂ is formed when Sb content exceeds the solid solubility limit of x = 0.02 in Cu_1.8S, all Cu_1.8–x Sb_x S bulk samples exhibit p-type conductivity characteristics. Benefitting from the synergistic phonon scattering effect by multiscale defects, such as point defects (${\rm{Sb}}_{{\rm{Cu}}}^{ \bullet\bullet }$, $ {\rm{V}}_{\rm{S}}^{ \bullet \bullet } $), nanopores, secondary phases (CuSbS₂), and dislocations, the thermal conductivity κ declines significantly from 1.76 W·m^–1·K^–1 (x = 0) to 0.99 W·m^–1·K^–1 at 723 K for the Cu_1.76Sb_0.04S sample. Finally, the peak dimensionless TE figure of merit (ZT ) value of 0.37 is achieved at 723 K for Cu_1.77Sb_0.03S resulting from a low thermal conductivity of 1.11 W·m^–1·K^–1 combining an appropriate power factor of 563 μW·m^–1·K^–2, which is 12% higher than that (0.33) of pristine Cu_1.8S. Although the Sb doped Cu_1.8S-based samples have lower thermal conductivity κ, the reduced power factor cannot be offset by reducing the thermal conductivity κ, so the TE figure of merit (ZT ) value is not significantly improved. Therefore, there is still much room for improving the performance of Sb doped Cu_1.8S-based thermoelectric material, and its thermoelectric performance can be further optimized through nano-second phase recombination, energy band engineering, and introducing multi-scale defects, etc. Our results suggest that the introduction of Sb into thermoelectric materials is an effective and convenient strategy to improve ZT value by reducing thermal conductivity κ.

Keywords:

作者及机构信息

北京科技大学材料科学与工程学院, 北京　100083

通信作者: 张波萍, bpzhang@ustb.edu.cn

基金项目: 国家重点研发计划(批准号: 2018YFB0703600)和国家自然科学基金(批准号: 11474176)资助的课题

Authors and contacts

School of Material Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China

Corresponding author: Zhang Bo-Ping, bpzhang@ustb.edu.cn

Funds: Project supported by the National Key Research and Development Program of China (Grant No. 2018YFB0703600) and the National Natural Science Foundation of China (Grant No. 11474176)

文章全文 : translate this paragraph

参考文献

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施引文献

图 1 Cu_1.8–x Sb_x S (x = 0, 0.005, 0.02, 0.03, 0.04)粉体样品的室温 XRD图谱(2θ = 20º−60º) (a)和(0 1 20)晶面放大峰(b)

Fig. 1. XRD patterns of the Cu_1.8–x Sb_x S powder samples (x = 0, 0.005, 0.02, 0.03, 0.04) at 2θ range of 20°−60° (a) and the enlarged (0 1 20) peaks (b).

下载: 全尺寸图片幻灯片

图 2 Cu_1.8–x Sb_x S (x = 0, 0.005, 0.02, 0.03, 0.04)块体样品的XRD图谱　(a) 2θ = 20º−60º; (b) 2θ = 31º−33º

Fig. 2. XRD patterns of the Cu_1.8–x Sb_x S bulk samples (x = 0.00, 0.005, 0.02, 0.03, 0.04) at 2θ range of 20º−60º (a) and 31º−33º (b).

下载: 全尺寸图片幻灯片

图 3 Cu_1.8–x Sb_x S块体样品的晶粒尺寸分布及断口FESEM照, 其中x取值分别为(a) x = 0, (b) x = 0.005, (c) x = 0.02, (d) x = 0.03, (e) x = 0.04; (f) 密度和相对密度随x变化图

Fig. 3. Grain size distributions of Cu_1.8–x Sb_x S bulks with FESEM images of the fractured surfaces in the inset at (a) x = 0.00, (b) x = 0.005, (c) x = 0.02, (d) x = 0.03, (e) x = 0.04; (f) density and relative density.

下载: 全尺寸图片幻灯片

图 4 Cu_1.8–x Sb_x S (x = 0, 0.005, 0.02, 0.03, 0.04)块体样品的电输运性能　(a) 电导率; (b) Seebeck系数; (c) 功率因子

Fig. 4. Temperature dependence of electrical transport properties for Cu_1.8–x Sb_x S (x = 0, 0.005, 0.02, 0.03, 0.04) bulks: (a) Electrical conductivity σ; (b) Seebeck coefficient α; (c) power factor PF.

下载: 全尺寸图片幻灯片

图 5 Cu_1.8–x Sb_x S (x = 0, 0.005, 0.02, 0.03, 0.04)块体样品的热输运性能　(a) 总热导率κ; (b) 洛伦兹常数L; (c) 电子热导率与总热导率的比值κ_e /κ

Fig. 5. Temperature dependence of thermal transport properties for Cu_1.8–x Sb_x S (x = 0, 0.005, 0.02, 0.03, 0.04) bulks: (a) Total thermal conductivity κ; (b) Lorenz number L; (c) the ratios of electronic thermal conductivity to total thermal conductivity (κ_e /κ).

下载: 全尺寸图片幻灯片

图 6 (a) Cu_1.8–x Sb_x S (x = 0, 0.005, 0.02, 0.03, 0.04)块体的ZT值; (b) 723 K时不同Cu_1.8S基材料的热电性能对比^{[18,21,34-37]}

Fig. 6. (a) Temperature dependence of ZT for Cu_1.8–x Sb_x S (x = 0, 0.005, 0.02, 0.03, 0.04) bulks; (b) comparisons of thermoelectric properties of different Cu_1.8S-based materials at 723 K^{[18,21,34-37]}.

下载: 全尺寸图片幻灯片

[1]	葛振华, 张波萍, 于昭新, 刘勇, 李敬锋 2012 物理学报 61 048401 Google Scholar Ge Z H, Zhang B P, Yu Z X, Liu Y, Li J F 2012 Acta Phys. Sin. 61 048401 Google Scholar
[2]	赵立东, 张波萍, 李敬锋, 刘玮书, 周敏 2007 稀有金属材料与工程 36 408 Google Scholar Zhao L D, Zhang B P, Li J F, Liu W S, Zhou M 2007 Rare Metal Mat. Eng. 36 408 Google Scholar
[3]	张贺, 骆军, 朱航天, 刘泉林, 梁敬魁, 饶光辉 2012 物理学报 61 086101 Google Scholar Zhang H, Luo J, Zhu H T, Liu Q Lin, Liang J K, Rao G H 2012 Acta Phys. Sin. 61 086101 Google Scholar
[4]	王作成, 李涵, 苏贤礼, 唐新峰 2011 物理学报 60 027202 Google Scholar Wang Z C, Li H, Su X L, Tang X F 2011 Acta Phys. Sin. 60 027202 Google Scholar
[5]	Snyder G J, E S Toberer 2008 Nat. Mater. 7 105 Google Scholar
[6]	Francis J D 1999 Science 285 703 Google Scholar
[7]	He J, Tritt T M 2017 Science 357 k9997 Google Scholar
[8]	Tan G, Zhao L, Kanatzidis M G 2016 Chem. Rev. 116 12123 Google Scholar
[9]	Zhu T, Liu Y, Fu C, Heremans J P, Snyder J G, Zhao X 2017 Adv. Mater. 29 1605884 Google Scholar
[10]	Liu Z, Mao J, Liu T, Chen G, Ren Z 2018 MRS. Bull. 43 181 Google Scholar
[11]	Liu Z, Sun J, Mao J, Zhu H, Ren W, Zhou J, Wang Z, Singh D J, Sui J, Chu C, Ren Z 2018 Proc. Natl. Acad. Sci. U. S. A. 115 5332 Google Scholar
[12]	Wang L, Li J, Zhang C, Ding T, Xie Y, Li Y, Liu F, Ao W, Zhang C 2020 J. Mater. Chem. A 8 1660 Google Scholar
[13]	Qiu P F, Zhu Y Q, Qin Y T, Shi X, Chen L D 2016 APL Mater. 4 104805 Google Scholar
[14]	Zhao L, Wang X, Fei F Y, Wang J, Cheng Z, Dou S, Wang J, Snyder G J 2015 J. Mater. Chem. A 3 9432 Google Scholar
[15]	Ge Z, Zhang B, Chen Y, Yu Z, Liu Y, Li J 2011 Chem. Commun. 47 12697 Google Scholar
[16]	Dennler G, Chmielowski R, Jacob S, Capet F, Roussel P, Zastrow S, Nielsch K, Opahle I, Madsen G K H 2014 Adv. Energy Mater. 4 1301581 Google Scholar
[17]	Qin P, Qian X, Ge Z H, Zheng L, Feng J, Zhao L D 2017 Inog. Chem. Front. 4 1192 Google Scholar
[18]	Ge Z, Liu X, Feng D, Lin J, He J 2016 Adv. Energy Mater. 6 1600607 Google Scholar
[19]	Ge Z H, Chong X, Feng D, Zhang Y X, Qiu Y, Xie L, Guan P W, Feng J, He J 2019 Mater. Today Phys. 8 71 Google Scholar
[20]	Zou L, Zhang B, Ge Z, Gao C, Zhang D, Liu Y 2013 Phys. Status Solidi A. 210 2550 Google Scholar
[21]	Qin P, Ge Z, Feng J 2017 J. Alloys Compd. 696 782 Google Scholar
[22]	Yao Y, Zhang B, Pei J, Han Y, Zhou M 2016 Ceram. Int. 42 17518 Google Scholar
[23]	Liang D, Ge Z, Li H, Zhang B, Li F 2017 J. Alloys Compd. 708 169 Google Scholar
[24]	Ge Z, Zhang Y, Song D, Chong X, Qin P, Zheng F, Feng J, Zhao L 2018 J. Mater. Chem. A 6 14440 Google Scholar
[25]	Tang H, Zhuang H, Cai B, Asfandiyar A, Dong J, Sun F, Li J 2019 J. Mater. Chem. C 7 4026 Google Scholar
[26]	Bayikadi K S, Wu C T, Chen L, Chen K, Chou F, Sankar R 2020 J. Mater. Chem A 8 5332 Google Scholar
[27]	Chen T, Zhang K, Wang H, Su W, Mehmood F, Wang T, Zhai J, Wang X, Huo T, Wang C 2020 J. Mater. Chem. C 8 1679 Google Scholar
[28]	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
[29]	Poudel B, Hao Q, Ma Y, Lan Y, Minnich A, Yu B, Yan X, Wang D, Muto A, Vashaee D, Chen X, Liu J, Dresselhaus M S, Chen G, Ren Z 2008 Science 320 634 Google Scholar
[30]	Li J, Zhang X, Chen Z, Lin S, Li W, Shen J, Witting I T, Faghaninia A, Chen Y, Jain A, Chen L, Snyder G J, Pei Y 2018 Joule 2 976 Google Scholar
[31]	Zhao L D, Wu H J, Hao S Q, Wu C I, Zhou X Y, Biswas K, He J Q, Hogan T P, Uher C, Wolverton C, Dravid V P, Kanatzidis M G 2013 Energy Environ. Sci. 6 3346 Google Scholar
[32]	Xu Q, Huang B, Zhao Y F, Yan Y F, Noufi R, Wei S H 2012 Appl. Phys. Lett. 100 061906 Google Scholar
[33]	Chakrabarti D J, Laughlin D E 1983 Bull. Alloy Phase Diagrams 4 254 Google Scholar
[34]	Tang C, Liang D, Li H, Luo K, Zhang B 2019 J. Adv. Ceram. 8 209 Google Scholar
[35]	Zhou Y, Ge Z, Gan G, Song P, Feng J 2019 Solid State Sci. 95 105953 Google Scholar
[36]	Zhang Y, Ma Z, Ge Z, Qin P, Zheng F, Feng J 2018 J. Alloys Compd. 764 738 Google Scholar
[37]	Qin P, Ge Z, Feng J 2017 J. Mater. Res. 32 3029 Google Scholar

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[20]	闫文胜, 范江玮, 李玉芝, 崔宏滨, 刘文汉, 张新夷, 韦世强. 机械合金化Fe100-xCux体系的X射线吸收精细结构研究. 物理学报, 2001, 50(4): 758-764. doi: 10.7498/aps.50.758

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Cu_1.8–x Sb_x S热电材料的相结构与电热输运性能