Realizing high thermoelectric performance in SnSe<sub>2 </sub><i>via</i> intercalating Cu

Li Cai-Yun; He Wen-Ke; Wang Dong-Yang; Zhang Xiao; Zhao Li-Dong

doi:10.7498/aps.70.20211444

Abstract

SnSe, a layered material with intrinsic low thermal conductivity, is reported to have excellent thermoelectric properties. SnSe₂ has a similar structure to SnSe, but the SnSe₂ has a low electrical transport, resulting in a poor thermoelectric performance, and the intrinsic SnSe₂ has a maximum ZT value of only ~ 0.09 at 773 K. In this work, SnSe_1.98Br_0.02-y%Cu (y = 0, 0.50, 0.75, 1.0) bulk materials are synthesized by the melting method combined with spark plasma sintering (SPS) based on the carrier concentration improved through Br doping. In the SnSe₂ materials with van der Waals chemical bonding between layers, the synergistic effects of intercalating Cu on the thermoelectric properties are investigated. On the one hand, the extra Cu not only provides additional electrons but also can be embedded stably in the van der Waals gap and form an intercalated structure, which is beneficial to the charge transfer in or out of the layers, and thus synergistically improving the carrier concentration and carrier mobility. On the other hand, owing to the dynamic Cu doping, the increase of carrier concentration compensates for the decrease of carrier mobility caused by carrier-carrier scattering, which maintains the high electrical transport properties at high temperature. The present results show that at room temperature, the power factors along the parallel and perpendicular to the SPS (//P and ⊥P) sintering directions increase from ~0.65 and ~0.98 µW·cm^–1·K^–2 for intrinsic SnSe₂ to ~10 and ~19 μW·cm^–1·K^–2 for SnSe_1.98Br_0.02-0.75%Cu samples, respectively. Finally, at 773 K, the maximum ZT value of ~0.8 is achieved along the ⊥P direction. This study proves that the SnSe₂ greatly promises to become an excellent thermoelectric material.

Keywords:

Authors and contacts

1.
School of Materials Science and Engineering, Beihang University, Beijing 100191, China
2.
Hangzhou Innovation Institute, Beihang University, Hangzhou 310056, China

Corresponding author: Zhang Xiao, zhang_xiao@buaa.edu.cn ; Zhao Li-Dong, zhaolidong@buaa.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51772012, 52002042, 52002011), the National Key R&D Program of China (Grant Nos. 2018YFA0702100, 2018YFB0703600), the Natural Science Foundation of Beijing, China (Grant No. JQ18004), the 111Project (Grant No. B17002), the National Postdoctoral Program for Innovative Talents of China (Grant No. BX20200028), the China Postdoctoral Science Foundation (Grant No. 2021M690280), the Natural Science Foundation of Chongqing, China (Grant No. cstc2019jcyj-msxmX0554), the High-Performance Computing (HPC) Resources at Beihang University, China, and the National Science Fund for Distinguished Young Scholars of China (Grant No. 51925101).

[1]	Zhang X, Zhao L D 2015 J. Materiomics 1 92 Google Scholar
[2]	Li J F, Liu W S, Zhao L D, Zhou M 2010 NPG Asia Mater. 2 152 Google Scholar
[3]	赵立东, 张德培, 赵勇 2015 西华大学学报 (自然科学版) 34 1 Google Scholar Zhao L D, Zhang D P, Zhao Y 2015 J. Xihua Univ. (Nat. Sci. Ed. ) 34 1 Google Scholar
[4]	Xiao Y, Zhao L D 2020 Science 367 1196 Google Scholar
[5]	蒋俊, 许高杰, 崔平, 陈立东 2005 55 4849 Google Scholar Jiang J, Xu G J, Cui P, Chen L D 2005 Acta Phys. Sin. 55 4849 Google Scholar
[6]	郑丽仙, 胡剑峰, 骆军 2020 69 247102 Google Scholar Zheng L X, Hu J F, Luo J 2020 Acta Phys. Sin. 69 247102 Google Scholar
[7]	赵英浩, 张瑞, 张波萍, 尹阳, 王明军, 梁豆豆 2021 70 128401 Google Scholar Zhao Y H, Zhang R, Zhang B P, Yin Y, Wang M J, Liang D D 2021 Acta Phys. Sin. 70 128401 Google Scholar
[8]	Xiao Y, Wang D Y, Zhang Y, Chen C G, Zhang S X, Wang K D, Wang G T, Pennycook S J, Snyder G J, Wu H J, Zhao L D 2020 J. Am. Chem. Soc 142 4051 Google Scholar
[9]	He W K, Wang D Y, Jun W H, et al. 2019 Science 365 1418 Google Scholar
[10]	Zhao L D, Chang C, Tan G J, Kanatzidis M G 2016 Energy Environ. Sci. 9 3044 Google Scholar
[11]	Tan G J, Zhao L D, Kanatzidis M G 2016 Chem. Rev. 116 12123 Google Scholar
[12]	Zhao L D, Lo S H, Zhang Y, Sun H, Tan G, Uher C, Wolverton C, Dravid V P, Kanatzidis M G 2014 Nature 508 373 Google Scholar
[13]	Chang C, Wu M H, He D S, Pei Y L, Wu C F, Wu X F, Yu H L, Zhu F Y, Wang K D, Chen Y, Huang L, Li J F, He J Q, Zhao L D 2018 Science 360(SI) 778
[14]	Qin B C, Wang D Y, Liu X X, Qin Y X, Dong J F, Luo J F, Li J W, Liu W, Tan G J, Tang X F, Li J F, He J, Zhao L D 2021 Science 373 556 Google Scholar
[15]	Sun J, Liu S, Wang C, Bai Y, Chen G, Luo Q, Ma F 2020 Appl. Surf. Sci. 510 145478 Google Scholar
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[17]	Pham A T, Vu T H, Chang C, Trinh T L, Lee J E, Ryu H, Hwang C, Mo S K, Kim J, Zhao L D, Duong A T, Cho S 2020 ACS Appl. Energy Mater. 3 10787 Google Scholar
[18]	Shu Y J, Su X L, Xie H Y, Zheng G, Liu W, Yan Y G, Luo T T, Yang X, Wang D Y, Uher C, Tang X F 2018 ACS Appl. Mater. Interfaces 10 15793 Google Scholar
[19]	Liu C Y, Huang Z W, Wang D H, Wang X X, Miao L, Wang X Y, Wu S H, Toyama N, Asaka T, Chen J L, Nishibori E, Zhao L D 2019 J. Mater. Chem. A 7 9761 Google Scholar
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[25]	Qin B C, Wang D Y, He W K, Zhang Y, Wu H J, Pennycook S J, Zhao L D 2018 J. Am. Chem. Soc 141 1141 Google Scholar
[26]	Blöchl P E 1994 Phys. Rev. B 50 17953 Google Scholar
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[28]	John P P, Kieron B, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865 Google Scholar
[29]	Zhou C, Yu Y, Zhang X, Cheng Y, Xu J, Lee Y K, Yoo B, Cojocaru‐Mirédin O, Liu G, Cho S P, Wuttig M, Hyeon T, Chung In 2019 Adv. Funct. Mater. 30 1908405 Google Scholar
[30]	Savin A, Jepsen O, Flad J, Andersen O K, Preuss H, von Schnering H G 1992 Angew. Chem. Int. Ed. 31 187 Google Scholar
[31]	Sun B Z, Ma Z J, He C, Wu K C 2015 Phys. Chem. Chem. Phys. 17 29844 Google Scholar
[32]	Qian X, Wang D Y, Zhang Y, Wu H J, Pennycook S J, Zheng L, Poudeu P F P, Zhao L D 2020 J. Mater. Chem. A 8 5699 Google Scholar
[33]	Li C Y, He W K, Wang D Y, Zhao L D 2021 Chin. Phys. B 30 067101 Google Scholar
[34]	Yamamoto M, Ohta H, Koumoto K 2007 Appl. Phys. Lett. 90 072101 Google Scholar
[35]	Zhao L D, Zhang B P, Liu W S, Zhang H L, Li J F 2008 J. Solid State Chem. 181 3278 Google Scholar
[36]	Pei Y L, He J Q, Li J F, Li F, Liu Q J, Pan W, Barreteau C, Berardan D, Dragoe N, Zhao L D 2013 NPG Asia Mater. 5 e47 Google Scholar
[37]	Ge Z H, Song D, Chong X, Zheng F, Jin L, Qian X, Zheng L, Dunin-Borkowski R E, Qin P, Feng J, Zhao L D 2017 J. Am. Chem. Soc 139 9714 Google Scholar

Cited By

图 1 SnSe_1.98Br_0.02-y%Cu (y = 0, 0.50, 0.75, 1.00)的 (a) 室温XRD和(b) 晶格常数

Figure 1. (a) XRD patterns and (b) lattice parameters for SnSe_1.98Br_0.02-y%Cu (y = 0, 0.50, 0.75, 1.00).

DownLoad: Full-Size Img PowerPoint

图 2 SnSe_1.98Br_0.02-y%Cu沿//P和⊥P方向　(a), (b) 电导率; (c), (d) Seebeck系数; (e), (f) 功率因子

Figure 2. (a), (b) Electrical conductivity, (c), (d) Seebeck coefficient and (e), (f) power factor for the samples of SnSe_1.98Br_0.02-y%Cu samples along the //P and ⊥P directions.

DownLoad: Full-Size Img PowerPoint

图 3 (a) SnSe_1.98Br_0.02-y%Cu样品沿//P和⊥P方向的载流子浓度和载流子迁移率; (b) SnSe_2–xBr_x和SnSe_1.98Br_0.02-y%Cu的Seebeck系数随载流子浓度的变化; SnSe_1.98Br_0.02 ^[29]和SnSe_1.98Br_0.02-0.75%Cu样品的(c)载流子浓度和(d)载流子迁移率随温度的变化

Figure 3. (a) Carrier concentration and carrier mobility at room temperature for the samples of SnSe_1.98Br_0.02-y%Cu along the //P and ⊥P directions; (b) Seebeck coefficient as function of carrier concentration; (c) carrier concentration and (d) carrier mobility as function of temperature for SnSe_1.98Br_0.02^[29] and SnSe_1.98Br_0.02-0.75%Cu samples.

DownLoad: Full-Size Img PowerPoint

图 4 (a) Sn₁₈CuSe₃₆沿c轴方向投影的电子局域函数(ELF); (b) Sn₁₈CuSe₃₆的差分电荷密度

Figure 4. (a) Electron localization function (ELF) projected along the c-axis and (b) differential charge density of Sn₁₈CuSe₃₆.

DownLoad: Full-Size Img PowerPoint

图 5 SnSe_1.98Br_0.02-y%Cu沿//P和⊥P的总热导率((a), (b))和晶格热导率((c), (d))

Figure 5. The temperature dependence of thermal conductivity along the //P and⊥P directions for SnSe_1.98Br_0.02-y%Cu: (a), (b) Total thermal conductivity; (c), (d) lattice thermal conductivity.

DownLoad: Full-Size Img PowerPoint

图 6 SnSe_1.98Br_0.02-y%Cu的随温度变化的ZT值沿(a) //P方向和(b) ⊥P方向

Figure 6. Temperature dependent ZT values along the (a) //P and (b) ⊥P directions for SnSe_1.98Br_0.02-y%Cu samples.

DownLoad: Full-Size Img PowerPoint

map

[1]	Zhang X, Zhao L D 2015 J. Materiomics 1 92 Google Scholar
[2]	Li J F, Liu W S, Zhao L D, Zhou M 2010 NPG Asia Mater. 2 152 Google Scholar
[3]	赵立东, 张德培, 赵勇 2015 西华大学学报 (自然科学版) 34 1 Google Scholar Zhao L D, Zhang D P, Zhao Y 2015 J. Xihua Univ. (Nat. Sci. Ed. ) 34 1 Google Scholar
[4]	Xiao Y, Zhao L D 2020 Science 367 1196 Google Scholar
[5]	蒋俊, 许高杰, 崔平, 陈立东 2005 55 4849 Google Scholar Jiang J, Xu G J, Cui P, Chen L D 2005 Acta Phys. Sin. 55 4849 Google Scholar
[6]	郑丽仙, 胡剑峰, 骆军 2020 69 247102 Google Scholar Zheng L X, Hu J F, Luo J 2020 Acta Phys. Sin. 69 247102 Google Scholar
[7]	赵英浩, 张瑞, 张波萍, 尹阳, 王明军, 梁豆豆 2021 70 128401 Google Scholar Zhao Y H, Zhang R, Zhang B P, Yin Y, Wang M J, Liang D D 2021 Acta Phys. Sin. 70 128401 Google Scholar
[8]	Xiao Y, Wang D Y, Zhang Y, Chen C G, Zhang S X, Wang K D, Wang G T, Pennycook S J, Snyder G J, Wu H J, Zhao L D 2020 J. Am. Chem. Soc 142 4051 Google Scholar
[9]	He W K, Wang D Y, Jun W H, et al. 2019 Science 365 1418 Google Scholar
[10]	Zhao L D, Chang C, Tan G J, Kanatzidis M G 2016 Energy Environ. Sci. 9 3044 Google Scholar
[11]	Tan G J, Zhao L D, Kanatzidis M G 2016 Chem. Rev. 116 12123 Google Scholar
[12]	Zhao L D, Lo S H, Zhang Y, Sun H, Tan G, Uher C, Wolverton C, Dravid V P, Kanatzidis M G 2014 Nature 508 373 Google Scholar
[13]	Chang C, Wu M H, He D S, Pei Y L, Wu C F, Wu X F, Yu H L, Zhu F Y, Wang K D, Chen Y, Huang L, Li J F, He J Q, Zhao L D 2018 Science 360(SI) 778
[14]	Qin B C, Wang D Y, Liu X X, Qin Y X, Dong J F, Luo J F, Li J W, Liu W, Tan G J, Tang X F, Li J F, He J, Zhao L D 2021 Science 373 556 Google Scholar
[15]	Sun J, Liu S, Wang C, Bai Y, Chen G, Luo Q, Ma F 2020 Appl. Surf. Sci. 510 145478 Google Scholar
[16]	Wang H F, Gao Y, Liu G 2017 RSC Adv. 7 8098 Google Scholar
[17]	Pham A T, Vu T H, Chang C, Trinh T L, Lee J E, Ryu H, Hwang C, Mo S K, Kim J, Zhao L D, Duong A T, Cho S 2020 ACS Appl. Energy Mater. 3 10787 Google Scholar
[18]	Shu Y J, Su X L, Xie H Y, Zheng G, Liu W, Yan Y G, Luo T T, Yang X, Wang D Y, Uher C, Tang X F 2018 ACS Appl. Mater. Interfaces 10 15793 Google Scholar
[19]	Liu C Y, Huang Z W, Wang D H, Wang X X, Miao L, Wang X Y, Wu S H, Toyama N, Asaka T, Chen J L, Nishibori E, Zhao L D 2019 J. Mater. Chem. A 7 9761 Google Scholar
[20]	Xu P P, Fu T Z, Xin J Z, Liu Y T, Ying P T, Zhao X B, Pan H G, Zhu T J 2017 Sci. Bull. 62 1663 Google Scholar
[21]	Luo Y B, Zheng Y, Luo Z Z, Hao S Q, Du C F, Liang Q H, Li Z, Khor K A, Hippalgaonkar K, Xu J W, Yan Q Y, Wolverton C, Kanatzidis M G 2018 Adv. Energy Mater. 8 1702167 Google Scholar
[22]	施先珍 2014 硕士学位论文 (武汉: 武汉理工大学) Shi X Z 2014 M. S. Thesis (Wuhan: Wuhan University of Technology) (in Chinese)
[23]	Sun G L, Qin X Y, Li D, Zhang J, Ren B J, Zou T H, Xin H X, Paschen S B, Yan X L 2015 J. Alloys Compd. 639 9 Google Scholar
[24]	Xiao Y, Wu H J, Li W, Yin M J, Pei Y L, Zhang Y, Fu L W, Chen Y X, Pennycook S J, Huang L, He J Q, Zhao L D 2017 J. Am. Chem. Soc 139 18732 Google Scholar
[25]	Qin B C, Wang D Y, He W K, Zhang Y, Wu H J, Pennycook S J, Zhao L D 2018 J. Am. Chem. Soc 141 1141 Google Scholar
[26]	Blöchl P E 1994 Phys. Rev. B 50 17953 Google Scholar
[27]	Kresse G, Furthmüller J 1996 Phys. Rev. B 54 11169 Google Scholar
[28]	John P P, Kieron B, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865 Google Scholar
[29]	Zhou C, Yu Y, Zhang X, Cheng Y, Xu J, Lee Y K, Yoo B, Cojocaru‐Mirédin O, Liu G, Cho S P, Wuttig M, Hyeon T, Chung In 2019 Adv. Funct. Mater. 30 1908405 Google Scholar
[30]	Savin A, Jepsen O, Flad J, Andersen O K, Preuss H, von Schnering H G 1992 Angew. Chem. Int. Ed. 31 187 Google Scholar
[31]	Sun B Z, Ma Z J, He C, Wu K C 2015 Phys. Chem. Chem. Phys. 17 29844 Google Scholar
[32]	Qian X, Wang D Y, Zhang Y, Wu H J, Pennycook S J, Zheng L, Poudeu P F P, Zhao L D 2020 J. Mater. Chem. A 8 5699 Google Scholar
[33]	Li C Y, He W K, Wang D Y, Zhao L D 2021 Chin. Phys. B 30 067101 Google Scholar
[34]	Yamamoto M, Ohta H, Koumoto K 2007 Appl. Phys. Lett. 90 072101 Google Scholar
[35]	Zhao L D, Zhang B P, Liu W S, Zhang H L, Li J F 2008 J. Solid State Chem. 181 3278 Google Scholar
[36]	Pei Y L, He J Q, Li J F, Li F, Liu Q J, Pan W, Barreteau C, Berardan D, Dragoe N, Zhao L D 2013 NPG Asia Mater. 5 e47 Google Scholar
[37]	Ge Z H, Song D, Chong X, Zheng F, Jin L, Qian X, Zheng L, Dunin-Borkowski R E, Qin P, Feng J, Zhao L D 2017 J. Am. Chem. Soc 139 9714 Google Scholar

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Realizing high thermoelectric performance in SnSe₂via intercalating Cu

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Corresponding author: Zhang Xiao, zhang_xiao@buaa.edu.cn ; Zhao Li-Dong, zhaolidong@buaa.edu.cn

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Realizing high thermoelectric performance in SnSe2 via intercalating Cu

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Corresponding author: Zhang Xiao, zhang_xiao@buaa.edu.cn ; Zhao Li-Dong, zhaolidong@buaa.edu.cn

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Realizing high thermoelectric performance in SnSe₂via intercalating Cu