多组元掺杂提升Cu<sub>3</sub>SbSe<sub>4</sub>基固溶体的热电性能

王莫凡; 应鹏展; 李勰; 崔教林

doi:10.7498/aps.70.20202094

摘要

Cu₃SbSe₄是一种具有黄铜矿结构的三元p-型半导体材料, 在热电领域颇受重视. 本次工作采用在Cu₃SbSe₄中先掺杂Sn与S, 然后再掺杂Ga₂Te₃这一多组元掺杂方式, 通过能带及晶体结构计算, 了解多组元掺杂后热电性能提升的结构因素. 能带计算表明, 共掺杂Sn与S后, 禁带区域萌生出杂质带, 导致材料的载流子浓度(n_H)和电学性能大幅提高. 在691 K时, 功率因子(PF)从本征的5.2 μW·cm^–1·K^–2增大到13.0 μW·cm^–1·K^–2. 虽然Ga占位在Sb或Te占位在Se位置对能带结构作用甚少, 但四面体[SbSe₄]和[SeCu₃Sb]的键长和键角发生了改变, 从而产生了明显的局部点阵畸变. 因此, 在691 K时, 晶格热导率(κ_L)从1.23 W·K^–1·m^–1降低到0.81 W·K^–1·m^–1, 有效地抑制了总热导率(κ)的提高. 最终, 材料的最大热电优值(ZT)为0.64, 而本征Cu₃SbSe₄的ZT值为0.26.

关键词:

Abstract

Cu₃SbSe₄, one of the ternary p-type semiconductor materials with chalcopyrite structure, has aroused much interest in thermoelectrics due to its inherent large effective mass and narrow bandgap. Therefore, many researches have been done, which cover the single and/or multi-element doping to manipulate its band structure and introduce the point defects. Although great achievements have been made in recent years, the mechanism in Cu₃SbSe₄ with respect to the phonon and electronic transport properties needs further investigating. In this work, first, Sn and S are co-doped into Cu₃SbSe₄ and then the resulting compound is alloyed with Ga₂Te₃, to improve its TE performance and understand the mechanism by calculating the band structure and crystal structure. The calculation of band structure reveals that an impurity band is created within the bandgap after co-doping Sn and S due to their contributions to the density of the states (DOS), which is directly responsible for the significant improvement in carrier concentration (n_H) and electrical property. Therefore, the power factor (PF) is enhanced from 0.52 × 10^–3 to 1.3 × 10^–3 W·m^–1·K^–2. Although the effect associated with the Ga (Te) residing at Sb (Se) sites on the band structure is limited due to the fact that both the single Ga- and single Te-doped band structure remain almost unchanged, the structural parameters (bond lengths and angles) of the polyhedrons [SeCu₃Sb] and [SbSe₄] before and after Te and Ga residing at Se and Sb sites respectively change remarkably. This yields the significant distortion of local lattice structure on an atomic scale. Therefore, the phonon scattering is enhanced and the lattice thermal conductivity (κ_L) decreases from 1.23 to 0.81 W·K^–1·m^–1 at 691 K. The reduction in κ_L prevents the total thermal conductivity (κ) from being enhanced rapidly. As a consequence, the highest ZT value of 0.64 is attained, which is much higher than that of the pristine Cu₃SbSe₄ (ZT = 0.26). In addition, we not only present a synergistic strategy to separately optimize the phonon and electronic properties, but also fully elaborate its mechanism and better understand that this strategy is an effective way to improve the TE performance of the Cu₃SbSe₄-based solid solutions.

Keywords:

作者及机构信息

1.
中国矿业大学材料科学与工程学院, 徐州　221116

2.
宁波工程学院材料科学与化学工程学院, 宁波　315211

通信作者: 应鹏展, ypz3889@cumt.edu.cn ; 崔教林, cuijiaolin@163.com

基金项目: 国家自然科学基金(批准号: 51671109)资助的课题

Authors and contacts

1.
School of Materials Science and Engineering, China University of Mining and Technology, Xuzhou 221116, China

2.
School of Materials and Chemical Engineering, Ningbo University of Technology, Ningbo 315211, China

Corresponding author: Ying Peng-Zhan, ypz3889@cumt.edu.cn ; Cui Jiao-Lin, cuijiaolin@163.com

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 51671109)

文章全文 : translate this paragraph

参考文献

[1]	Wei T, Wang H, Gibbs Z, Wu C, Snyder G J, Li J 2014 J. Mater. Chem. A 2 13527 Google Scholar
[2]	Zhang D, Yang J Y, Jiang Q H, Zhou Z W, Li X, Xin J W, Basit A, Ren Y Y, He X, Chu W J, Hou J D 2017 ACS Appl. Mater. Interfaces 9 28558 Google Scholar
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[18]	Li D, Li R, Qin X Y, Zhang J, Song C J, Wang L, Xin H X 2013 CrystEngComm 15 7166 Google Scholar
[19]	Li D, Ming H W, Li J M, Jabar B, Xu W, Zhang J, Qin X Y 2020 ACS Appl. Mater. Interfaces 12 3886 Google Scholar
[20]	Xie D D, Zhang B, Zhang A J, Chen Y J, Yan Y C, Yang H Q, Wang G W, Wang G Y, Han H D, Han G, Lu X, Zhou X Y 2018 Nanoscale 10 14546 Google Scholar
[21]	Garcia G, Palacios P, Cabot A, Wahnon P 2018 Inorg. Chem. 57 7321 Google Scholar
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[25]	Min L, Ying P Z, Li X, Cui J L 2020 J. Phys. D: Appl. Phys. 53 075304 Google Scholar
[26]	Kurosaki K, Matsumoto H, Charoenphakdee A, Yamanaka S, Ishimaru M, Hirotsu Y 2008 Appl. Phys. Lett. 93 012101 Google Scholar
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[35]	Zhao L L, Lin N M, Han Z K, Li X, Wang H Y, Cui J L 2019 Adv. Electron. Mater 5 1900485 Google Scholar
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[37]	Cui J L, He T T, Han Z K, Liu X L, Du Z L 2018 Sci. Rep. 8 8202 Google Scholar
[38]	Do D T, Mahanti S D 2014 J. Phys. Chem. Solids 75 477 Google Scholar
[39]	Han M K, Hoang K, Kong H J, Pcionek R, Uher C, Paraskevopoulos K M, Mahanti S D, Kanatzidis M G 2008 Chem. Mater. 20 3512 Google Scholar
[40]	Heremans J P, Wiendlocha B, Chamoire A M 2012 Energy Environ. Sci. 5 5510 Google Scholar
[41]	Wiendlocha B, Vaney J B, Candolfi C, Dauscher A, Lenoir B, Tobola J 2018 Phys. Chem. Chem. Phys. 20 12948 Google Scholar
[42]	Li M, Luo Y, Cai G M, Li X, Li X Y, Han Z K, Lin X Y, Sarker D, Cui J L 2019 J. Mater. Chem. A 7 2360 Google Scholar
[43]	Zhang L, Zheng Q, Xie Y, Lan Z, Prezhdo O V, Saidi W A, Zhao J 2018 Nano Lett. 18 1592 Google Scholar
[44]	Pei Y Z, Wang H, Snyder G J 2012 Adv. Mater. 24 6125 Google Scholar
[45]	Jaffe J E, Zunger A 1984 Phys. Rev. B 29 1882 Google Scholar
[46]	Wu W, Li Y, Du Z, Meng Q, Sun Z, Ren W, Cui J 2013 Appl. Phys. Lett. 103 011905 Google Scholar
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施引文献

图 1 (a) (Cu₃Sb_0.9Sn_0.1Se_3.6S_0.4)_1–x(Ga₂Te₃)_x (x = 0~0.0175)的粉末XRD图谱; (b) 晶格结构常数a和c; (c) 四方相晶体结构变形参数η; (d) 内部点阵结构扭曲参数ψ

Fig. 1. (a) X-ray diffraction patterns of the powders (Cu₃Sb_0.9Sn_0.1Se_3.6S_0.4)_1–x(Ga₂Te₃)_x (x = 0~0.0175); (b) lattice constants a and c; (c) tetragonal deformation parameters η; (d) internal lattice distortion parameter ψ.

下载: 全尺寸图片幻灯片

图 2 三种不同占位材料的计算形成能(E_f)　(a) 本征Cu₂₄Sb₈Se₃₂ (E_f = 0), 作为比较对象; (b) Sn和S共掺杂的Cu₂₄Sb₇Sn₁Se₂₈S₄; (c) Ga占位在Sb位置(Cu₂₄Sb₇Ga₁Se₃₂); (d) Te 占位在Se位置(Cu₂₄Sb₈Se₃₁Te₁). E_f值均是相对于本征Cu₂₄Sb₈Se₃₂的形成能

Fig. 2. Formation energies (E_f) of three solid solutions with different element occupations. (a) Pristine Cu₂₄Sb₈Se₃₂ (E_f = 0) for comparidon; (b) Sn and S co-doped Cu₂₄Sb₇Sn₁Se₂₈S₄; (c) Ga residing at Sb site (Cu₂₄Sb₇Ga₁Se₃₂); (d) Te residing at Se site (Cu₂₄Sb₈Se₃₁Te₁). The E_f values are their corresponding formation energies in comparison to that of the pristine structure.

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图 3 各种材料的能带结构与态密度(DOS)　(a) Cu₂₄Sb₈Se₃₂; (b) Sn and S co-doped Cu₂₄Sb₇Sn₁Se₂₈S₄; (c) Ga doped Cu₂₄Sb₇Ga₁Se₃₂; (d) Te doped Cu₂₄Sb₈Se₃₁Te₁ compounds

Fig. 3. Band structures and the density of the states (DOS) of different materials: (a) Pristine Cu₂₄Sb₈Se₃₂; (b) Sn and S co-doped Cu₂₄Sb₇Sn₁Se₂₈S₄; (c) Ga doped Cu₂₄Sb₇Ga₁Se₃₂; (d) Te doped Cu₂₄Sb₈Se₃₁Te₁ compounds.

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图 4 Te和Ga分别占位在Se和Sb前后的多面体[SeCu₃Sb]和[SbSe₄]结构参数(键长和键角)

Fig. 4. Structural parameters (bond lengths and angles) of the polyhedrons [SeCu₃Sb] and [SbSe₄] before and after residing of Te and Ga at Se and Sb sites respectively.

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图 5 (a) 在室温下(Cu₃Sb_0.9Sn_0.1Se_3.6S_0.4)(Ga₂Te₃)_x (x = 0~0.0175)材料的霍尔载流子浓度(n_H)与Ga₂Te₃含量(x值)的关系; (b) 在室温下迁移率(μ)与Ga₂Te₃含量(x值)的关系

Fig. 5. (a) Hall carrier concentration (n_H) as a function of Ga₂Te₃ content (x value) at room temperature (RT) for (Cu₃Sb_0.9Sn_0.1Se_3.6S_0.4)(Ga₂Te₃)_x (x = 0~0.0175); (b) mobility (μ) as a function of Ga₂Te₃ content (x value) at RT.

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图 6 (Cu₃Sb_0.9Sn_0.1Se_3.6S_0.4)(Ga₂Te₃)_x (x = 0.01—0.015)材料的热电性能与温度的关系, 本征Cu₃SbSe₄的性能作为比较　(a) Seebeck 系数(α)与温度的关系; (b) 电导率(σ)与温度的关系; (c) 功率因子(PF) 与温度的关系; (d) 总热导率(κ)与温度的关系; (e) 晶格热导率(κ_L)与温度的关系; (f) 热电优值(ZT)与温度的关系

Fig. 6. TE performance of (Cu₃Sb_0.9Sn_0.1Se_3.6S_0.4)(Ga₂Te₃)_x (x = 0.01–0.015) as a function of temperature, and the TE performance of pristine Cu₃SbSe₄ is provided for comparison: (a) Seebeck coefficients as a function of temperature; (b) electrical conductivities as a function of temperature; (c) power factor (PF) as a function of temperature; (d) total thermal conductivities (κ) as a function of temperature; (e) lattice part (κ_L) as a function of temperature; (f) TE figure of merit (ZT) as a function of temperature.

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map

[1]	Wei T, Wang H, Gibbs Z, Wu C, Snyder G J, Li J 2014 J. Mater. Chem. A 2 13527 Google Scholar
[2]	Zhang D, Yang J Y, Jiang Q H, Zhou Z W, Li X, Xin J W, Basit A, Ren Y Y, He X, Chu W J, Hou J D 2017 ACS Appl. Mater. Interfaces 9 28558 Google Scholar
[3]	陈萝娜, 刘叶烽, 张继业, 杨炯, 邢娟娟, 骆军, 张文清 2017 66 167201 Google Scholar Chen L N, Liu Y F, Zhang J Y, Yang J, Xing J J, Luo J, Zhang W Q 2017 Acta Phys. Sin. 66 167201 Google Scholar
[4]	Zhao D G, Wu D, Bo L 2017 Energies 10 1524 Google Scholar
[5]	Chang C H, Chen C L, Chiu W T, Chen Y Y 2017 Mater. Lett. 186 227 Google Scholar
[6]	Zhang D, Yang J Y, Jiang Q H, Fu L W, Xiao Y, Luo Y B, Zhou Z W 2016 Mater. Des. 98 150 Google Scholar
[7]	Li Y Y, Qin X Y, Li D, Li X Y, Liu Y F, Zhang J, Song C J, Xin H X 2015 RSC Adv. 5 31399 Google Scholar
[8]	Yang C Y, Huang F Q, Wu L M, Xu K 2011 J. Phys. D: Appl. Phys. 44 295404 Google Scholar
[9]	Wang B Y, Zheng S Q, Wang Q, Li Z L, Li J, Zhang Z P, Wu Y, Zhu B S, Wang S Y, Chen Y X, Chen L Q, Chen Z G 2019 Mater. Res. Bull. 113 38 Google Scholar
[10]	Prasad K S, Rao A 2019 J. Mater. Sci. - Mater. Electron. 30 16596 Google Scholar
[11]	Wang B Y, Wang Y L, Zheng S Q, Liu S C, Li J, Chang S Y, An T, Sun W L, Chen Y X 2019 J. Alloys Compd. 806 676 Google Scholar
[12]	Skoug E J, Cain J D, Morelli D T 2011 Appl. Phys. Lett. 98 261911
[13]	Zhang D, Yang J Y, Bai H C, Luo Y B, Wang B, Hou S H, Li Z L, Wang S F 2019 J. Mater. Chem. A 7 17648 Google Scholar
[14]	Wang B Y, Zheng S Q, Chen Y X, Wu Y, Li J, Ji Z, Mu Y N, Wei Z B, Liang Q, Liang J X 2020 J. Phys. Chem. C 124 10336 Google Scholar
[15]	Li J M, Li D, Song C J, Wang L, Xin H X, Zhang J, Qin X Y 2019 Intermetallics 109 68 Google Scholar
[16]	Zhou T, Wang L J, Zheng S Q, Hong M, Fang T, Bai P P, Chang S Y, Cui W L, Shi X L, Zhao H Z, Chen Z G 2018 Nano Energy 49 221 Google Scholar
[17]	Wang B Y, Zheng S Q, Wang Q, Li Z L, Li J, Zhang Z P, Wu Y, Zhu B S, Wang S Y, Chen Y X, Chen L Q, Chen Z G 2020 Nano Energy 71 104658 Google Scholar
[18]	Li D, Li R, Qin X Y, Zhang J, Song C J, Wang L, Xin H X 2013 CrystEngComm 15 7166 Google Scholar
[19]	Li D, Ming H W, Li J M, Jabar B, Xu W, Zhang J, Qin X Y 2020 ACS Appl. Mater. Interfaces 12 3886 Google Scholar
[20]	Xie D D, Zhang B, Zhang A J, Chen Y J, Yan Y C, Yang H Q, Wang G W, Wang G Y, Han H D, Han G, Lu X, Zhou X Y 2018 Nanoscale 10 14546 Google Scholar
[21]	Garcia G, Palacios P, Cabot A, Wahnon P 2018 Inorg. Chem. 57 7321 Google Scholar
[22]	Do D T, Mahanti D 2015 J. Alloys Compd. 625 346 Google Scholar
[23]	Skoug E J, Cain J D, Morelli D T 2010 Appl. Phys. Lett. 96 181905 Google Scholar
[24]	Morelli D T, Slack G A 2006 High Thermal Conductivity Materials (New York: Springer) p37
[25]	Min L, Ying P Z, Li X, Cui J L 2020 J. Phys. D: Appl. Phys. 53 075304 Google Scholar
[26]	Kurosaki K, Matsumoto H, Charoenphakdee A, Yamanaka S, Ishimaru M, Hirotsu Y 2008 Appl. Phys. Lett. 93 012101 Google Scholar
[27]	Shen J W, Zhang X Y, Lin S Q, Li J, Chen Z W, Li W, Pei Y Z 2016 J. Mater. Chem. A 4 15464 Google Scholar
[28]	Guymont M, Tomas A, Guittard M 1992 Philos. Mag. A 66 133 Google Scholar
[29]	Kim H, Gibbs Z M, Tang Y, Wang H, Snyder G J 2015 APL Mater. 3 041506 Google Scholar
[30]	Blochl P E 1994 Phys. Rev. B 50 17953 Google Scholar
[31]	Kresse G, Furthmuller J 1996 Phys. Rev. B 54 11169 Google Scholar
[32]	Kresse G, Furthmuller J 1996 Comput. Mater. Sci. 6 15 Google Scholar
[33]	Pulay P 1980 Chem. Phys. Lett. 73 393 Google Scholar
[34]	Zeier W G, Pei Y Z, Pomrehn G, Day T, Heinz N, Heinrich C P, Snyder G J, Tremel W 2013 J. Am. Chem. Soc. 135 726 Google Scholar
[35]	Zhao L L, Lin N M, Han Z K, Li X, Wang H Y, Cui J L 2019 Adv. Electron. Mater 5 1900485 Google Scholar
[36]	Moreno E, Quintero M, Morocoima M, Quintero E, Grima P, Tovar R, Bocaranda P, Delgado G E, Contreras J E, Mora A E, Briceño J M, Godoy R A, Fernandez J L, Henao J A, Macías M A 2009 J. Alloys Compd. 486 212 Google Scholar
[37]	Cui J L, He T T, Han Z K, Liu X L, Du Z L 2018 Sci. Rep. 8 8202 Google Scholar
[38]	Do D T, Mahanti S D 2014 J. Phys. Chem. Solids 75 477 Google Scholar
[39]	Han M K, Hoang K, Kong H J, Pcionek R, Uher C, Paraskevopoulos K M, Mahanti S D, Kanatzidis M G 2008 Chem. Mater. 20 3512 Google Scholar
[40]	Heremans J P, Wiendlocha B, Chamoire A M 2012 Energy Environ. Sci. 5 5510 Google Scholar
[41]	Wiendlocha B, Vaney J B, Candolfi C, Dauscher A, Lenoir B, Tobola J 2018 Phys. Chem. Chem. Phys. 20 12948 Google Scholar
[42]	Li M, Luo Y, Cai G M, Li X, Li X Y, Han Z K, Lin X Y, Sarker D, Cui J L 2019 J. Mater. Chem. A 7 2360 Google Scholar
[43]	Zhang L, Zheng Q, Xie Y, Lan Z, Prezhdo O V, Saidi W A, Zhao J 2018 Nano Lett. 18 1592 Google Scholar
[44]	Pei Y Z, Wang H, Snyder G J 2012 Adv. Mater. 24 6125 Google Scholar
[45]	Jaffe J E, Zunger A 1984 Phys. Rev. B 29 1882 Google Scholar
[46]	Wu W, Li Y, Du Z, Meng Q, Sun Z, Ren W, Cui J 2013 Appl. Phys. Lett. 103 011905 Google Scholar
[47]	Jaffe J E, Zunger A 1983 Phys. Rev. B 28 5822 Google Scholar

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多组元掺杂提升Cu₃SbSe₄基固溶体的热电性能