Structure and thermoelectric performance of AgyIn3.33–y/3Se5 compounds

Zi Peng; Bai Hui; Wang Cong; Wu Yu-Tian; Ren Pei-An; Tao Qi-Rui; Wu Jin-Song; Su Xian-Li; Tang Xin-Feng

doi:10.7498/aps.71.20220179

Abstract

In this study, we find new Ag_yIn_3.33–y/3Se₅ compounds in Ag-In-Se system by static diffusion method combined with common X-ray diffraction and backscattering electron analysis. The crystal structure belongs to the trilateral system with the P3m1 space group, which features a two-dimensional layered structure. The unit cell is composed of 9-atom quantum layers arranged in the sequence of Se1-In1-Se2-In2-Se3-Ag/In3-Se4-In4-Se5, and in-between these layers are bonded by the weak van der Waals force. The sintered bulk samples show highly anisotropic transport properties and have an ultra-low lattice thermal conductivity along the direction parallel to sintering pressure about 0.15 W·m^–1·K^–1 at 873 K. The intrinsically ultra-low lattice thermal conductivity mainly comes from low phonon velocity and the strong coupling between low frequency optical phonon and acoustic phonons. The Ag_yIn_3.33–y/3Se₅ compounds behave as an n-type conduction. The electrical conductivity is 4×10⁴ S·m^–1 and the Seebeck coefficient is –80 μV·K^–1 at room temperature. Therefore, Ag_yIn_3.33–y/3Se₅ compounds show high electrical transport properties in a wide temperature range, and the power factor is around 5 μW·cm^–1·K^–2 in a range of 450–800 K. Owing to the ultra-low lattice thermal conductivity along the direction parallel to sintering pressure, Ag_0.407In_3.198Se₅ reaches a maximum ZT of 1.01 at 873 K and an average ZT of 0.45 at 300–850 K. The discovery of Ag_yIn_3.33–y/3Se₅ expands the n-type copper based chalcogenide and lays an important foundation for the application of copper based chalcogenide.

Keywords:

Authors and contacts

1.
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
2.
Nanostructure Research Center, Wuhan University of Technology, Wuhan 430070, China

Corresponding author: Su Xian-Li, suxianli@whut.edu.cn ; Tang Xin-Feng, tangxf@whut.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 Nos. 52122108, 51972256).

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References

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Cited By

图 1 (a) 三元Ag-In-Se系统示意相图; (b) 图(a)中红色区域的放大图

Figure 1. (a) Schematic ternary phase diagram of Ag-In-Se; (b) enlarged view of the red area in Fig.1 (a).

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图 2 (a) (Ag₂Se)_x(In₂Se₃)_100–x(x = 0—20)的粉末XRD图谱; (b) x = 0, 3.3, 5.3, 10.9, 13.6和16的背散射图片; (c) 所合成x = 0, 3.3, 5.3, 8.3, 10.9, 13.6和16的样品不同衬度区域电子能谱组成Ag/In比, 紫色虚线为合成样品名义组成线, 红色圆圈标出的为单相组成

Figure 2. (a) Powder XRD pattern of (Ag₂Se)_x(In₂Se₃)_100–x (x = 0–20); (b) backscattering electron (BSE) image of the samples with x = 0, 3.3, 5.3, 10.9, 13.6 and 16; (c) the ratio of Ag/In in x = 0, 3.3, 5.3, 8.3, 10.9, 13.6 and 16, the purple dotted line is the nominal composition line, and the red circle is marked as single-phase composition.

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图 3 (Ag₂Se)_x(In₂Se₃)_100–x (x = 10.9)样品的慢扫XRD(红色)(10°—90°), 精修得到的衍射峰(黑色), Bragg 峰位 (绿色), 衍射峰的差异(蓝色), R_p = 6.84%, R_wp = 9.31%.

Figure 3. Rietveld refinement of (Ag₂Se)_x(In₂Se₃)_100–x (x = 10.9), experimental (red point), calculated (black), Bragg position (green), defference (blue) R_p = 6.84%, R_wp = 9.31%.

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图 4 Ag_yIn_3.33–y/3Se₅的晶体结构图　(a) a轴投影; (b) c轴投影; (c) 单个晶胞的a轴投影; (d) 多面体的堆叠; (e) 以阳离子为中心的多面体

Figure 4. Crystal structure diagram of Ag_yIn_3.33–y/3Se₅: (a) a-axis projection; (b) c-axis projection; (c) a-axis projection of a single cell; (d) stacking of polyhedron; (e) cation centered polyhedron.

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图 5 (a)—(c) Ag_0.392In_3.203Se₅烧结块体自由断裂面的不同放大倍数的场发射扫描电镜照片

Figure 5. (a)–(c) Field emission scanning electron microscope images of freshly fractured surface for Ag_0.392In_3.203Se₅ bulk sample with different magnifications.

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图 6 (a) Ag_0.392In_3.203Se₅样品的低倍高角度环形暗场像(HAADF-STEM); (b)—(d) 图(a)中Ag-In-Se元素的能谱面扫描图(EDS-Map)

Figure 6. (a) HAADF-STEM (high-angle annular dark-field STEM) image of Ag_0.392In_3.203Se₅; (b)–(d) EDS elemental mapping of Ag, In, and Se of Fig. 6 (a).

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图 7 Ag_0.392In_3.203Se₅ 样品的微观图像　(a) [001]晶向的高倍高角度环形暗场像(HAADF-STEM); (b) 图(a)区域的选取电子衍射(SAED)和模拟的选取电子衍射(SAED); (c) [010] 晶向的高倍高角度环形暗场像(HAADF-STEM); (d) 图(c)区域的选取电子衍射(SAED)和模拟的选取电子衍射(SAED); (e), (f) 图(c)的染色放大图

Figure 7. Microstructure of Ag_0.392In_3.203Se₅: (a) High-magnification HAADF-STEM image along the [001]; (b) SAED pattern and calculation of (a); (c) high-magnification HAADF-STEM image along the [010]; (d) SAED pattern and calculation of (c); (e), (f) enlarged image of Fig.7 (c).

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图 A1 Ag_yIn_3.33–y/3Se₅ (y = 0.384, 0.392, 0.400, 0.407, 0.415)的XRD图谱

Figure A1. Powder XRD patterns of Ag_yIn_3.33–y/3Se₅ (y = 0.384, 0.392, 0.400, 0.407, 0.415).

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图 A2 Ag_yIn_3.33–y/3Se₅ (y = 0.384, 0.392, 0.400, 0.407, 0.415) 的背散射图片和元素面分布图

Figure A2. Backscattering electron (BSE) image and elemental distribution map of Ag_yIn_3.33–y/3Se₅ (y = 0.384, 0.392, 0.400, 0.407, 0.415).

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图 8 Ag_yIn_3.33–y/3Se₅ (y = 0.384, 0.392, 0.400, 0.407, 0.415)电输运性能　(a) 电导率; (b) 赛贝克系数; (c) 功率因子; (d) 单抛带模型计算载流子有效质量

Figure 8. Temperature dependences of (a) the electrical conductivity, (b) Seebeck coefficient, and (c) power factor for the Ag_yIn_3.33–y/3Se₅ (y = 0.384, 0.392, 0.400, 0.407, 0.415) samples; (d) Seebeck coefficients as a function of the charge carrier concentration at 300 K, where the dashed lines are Pisarenko plots based on the SPB model.

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图 9 Ag_yIn_3.33–y/3Se₅ (y = 0.384, 0.392, 0.400, 0.407, 0.415) 热输运性能和热电优值　(a) 热导率; (b) Ag_yIn_3.33–y/3Se₅ 与AgInSe₂^[35], AgInTe₂^[38], AgIn₅Se₈^[30]和CuInSe₂^[39]的晶格热导率; (c) Ag_yIn_3.33–y/3Se₅, AgInSe₂^[35], AgIn₅Se₈^[30], Ag_1.03In₅Se₈^[30], Ag_0.9Cd_0.1InSe₈^[35], Ag_1.02InSe₂^[35], Ag_1.6InSe_2.3^[40]的ZT值, 300—873 K; (d) 300—850 K的平均ZT_avg值

Figure 9. (a) The temperature-dependent of the total thermal conductivity for Ag_yIn_3.33–y/3Se₅; (b) the lattice thermal conductivity for Ag_yIn_3.33–y/3Se₅, AgInSe₂^[35], AgInTe₂^[38], AgIn₅Se₈^[30] and CuInSe₂^[39]; (c) merit ZT for Ag_yIn_3.33–y/3Se₅, AgInSe₂^[35], AgIn₅Se₈^[30], Ag_1.03In₅Se₈^[30], Ag_0.9Cd_0.1InSe₈^[35], Ag_1.02InSe₂^[35], Ag_1.6InSe_2.3^[40], at 300-873 K; (d) the average ZT at 300–850 K.

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图 10 Ag_0.392In_0.203Se₅样品的低温热容　(a) $C_{\rm p}/T^3\text-T$; (b) $ C_{\rm p}/T\text-T^2 $

Figure 10. (a) The relationship between $ C_{\rm p}/T^3 $and T, (b) C_p/T and T ²of Ag_0.392In_0.203Se₅.

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表 1 Ag_yIn_3.33–y/3Se₅样品的室温载流子浓度和迁移率

Table 1. The carrier concentration and Hall mobility of Ag_yIn_3.33–y/3Se₅ at room temperature.

Sample y = 0.384 y = 0.392 y = 0.400 y = 0.407 y = 0.415

μ_H / (cm²·V^–1·s^–1) 136.42 141.21 144.80 131.40 130.69
n_H /(10¹⁹ cm^–3) 1.88 1.70 1.68 1.93 1.85

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表 2 Ag_0.392In_0.203Se₅样品使用德拜-爱因斯坦模型拟合低温热容的参数

Table 2. Parameters obtained by fitting the experimental low-temperature heat capacity data to the Debye-Einstein model of Ag_0.392In_0.203Se₅.

Sample γ/
(mJ·mol^–1·K^–2) b/
(mJ·mol^–1·K^–4) A₁ θ_E1/K A₂ θ_E1/K θ_D/K

y = 0.392 0.02813 2.95 × 10^–4 13.43 40.18 57.01 82.63 164

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表 3 Ag_0.392In_0.203Se₅, AgInSe₂^[44]和AgIn₅Se₈^[30]的室温杨氏模量E、格林艾森常数常数γ对比

Table 3. Comparisons of Elastic properties and Grüneisen parameters at room temperature between Ag_0.392In_0.203Se₅, AgInSe₂^[44], and AgIn₅Se₈^[30].

Parameter Ag_0.392In_3.203Se₅ AgInSe₂ AgIn₅Se₈

v_l/(m·s^–1) 3058 3584 3778
v_s/(m·s^–1) 1527 1530 1803
v_a/(m·s^–1) 1713 1729 2028
E /GPa 35.0 52.5 50.6
γ 2.00 2.87 2.20

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map

[1]	Qin B, Wang D, Liu X, Qin Y, Dong J-F, Luo J, Li J-W, Liu W, Tan G, Tang X, Li J F, He J, Zhao L D 2021 Science 373 556 Google Scholar
[2]	范人杰, 江先燕, 陶奇睿, 梅期才, 唐颖菲, 陈志权, 苏贤礼, 唐新峰 2021 70 137102 Google Scholar Fan R J, Jiang X Y, Tao Q R, Mei Q C, Tang Y F, Chen Z Q, Su X L, Tang X F 2021 Acta Phys. Sin. 70 137102 Google Scholar
[3]	陶颖, 祁宁, 王波, 陈志权, 唐新峰 2018 67 197201 Google Scholar Tao Y, Qi N, Wang B, Chen Z Q, Tang X F 2018 Acta Phys. Sin. 67 197201 Google Scholar
[4]	Su X, Wei P, Li H, Liu W, Yan Y, Li P, Su C, Xie C, Zhao W, Zhai P, Zhang Q, Tang X, Uher C 2017 Adv. Mater. 29 23 Google Scholar
[5]	Deng R, Su X, Hao S, Zheng Z, Zhang M, Xie H, Liu W, Yan Y, Wolverton C, Uher C, Kanatzidis M G, Tang X 2018 Energy Environ. Sci. 11 1520 Google Scholar
[6]	Tao Q, Deng R, Li J, Yan Y, Su X, Poudeu P F P, Tang X 2020 ACS Appl. Mater. Interfaces 12 26330 Google Scholar
[7]	Tang X, Li Z, Liu W, Zhang Q, Uher C 2022 Interdiscip. Mater. 1 88 Google Scholar
[8]	Chen Z G, Shi X, Zhao L-D, Zou J 2018 Prog. Mater. Sci. 97 283 Google Scholar
[9]	Mangavati S, Pal A, Rao A, Jiang Z Z, Kuo Y K 2022 J. Phys. Chem. Solids. 160 110301 Google Scholar
[10]	Zhao X, Ning S, Qi N, Li Y, Dong Y, Zhang H, Liu J, Ye B, Chen Z 2021 ACS Appl. Mater. Interfaces 13 58936 Google Scholar
[11]	Zhang J, Zhu T, Zhang C, Yan Y, Tan G, Liu W, Su X, Tang X 2021 J. Alloy. Compd. 881 160639 Google Scholar
[12]	Zhang Q, Ti Z, Zhu Y, Zhang Y, Cao Y, Li S, Wang M, Li D, Zou B, Hou Y, Wang P, Tang G 2021 ACS Nano. 15 19345 Google Scholar
[13]	Zhang R, Pei J, Shan Z, Zhou W, Wu Y, Han Z, Zhao Y H, Li J F, Ge Z H, Zhang B P 2022 Chem. Eng. J. 429 132275 Google Scholar
[14]	杨枭, 苏贤礼, 鄢永高, 唐新峰 2021 无机材料学报 36 75 Google Scholar Yang X, Su X L, Yan Y G, Tang X F 2021 J. Inorg. Mater. 36 75 Google Scholar
[15]	Cao Y, Bai H, Li Z, Zhang Z, Tang Y, Su X, Wu J, Tang X 2021 ACS Appl. Mater. Interfaces 13 43134 Google Scholar
[16]	Su X, Hao S, Bailey T P, Wang S, Hadar I, Tan G, Song T B, Zhang Q, Uher C, Wolverton C, Tang X, Kanatzidis M G 2018 Adv. Energy Mater. 8 1800659 Google Scholar
[17]	杨东旺, 罗婷婷, 苏贤礼, 吴劲松, 唐新峰 2021 无机材料学报 36 991 Google Scholar Yang D W, Luo T T, Su X L, Wu J S, Tang X F 2021 J. Inorg. Mater. 36 991 Google Scholar
[18]	Cai S, Hao S, Luo Y, Su X, Luo Z-Z, Hu X, Wolverton C, Dravid V P, Kanatzidis M G 2020 Chem. Mater. 32 3561 Google Scholar
[19]	Ma N, Li F, Li J G, Liu X, Zhang D B, Li Y Y, Chen L, Wu L M 2021 J. Am. Chem. Soc. 143 18490 Google Scholar
[20]	Xia Y, Ozolins V, Wolverton C 2020 Phys. Rev. Lett. 125 085901 Google Scholar
[21]	Chen X, Carrete J, Sullivan S, van Roekeghem A, Li Z, Li X, Zhou J, Mingo N, Shi L 2019 Phys. Rev. Lett. 122 185901 Google Scholar
[22]	Zhang H, Liu H, Wei K, Kurakevych O O, Le Godec Y, Liu Z, Martin J, Guerrette M, Nolas G S, Strobel T A 2017 Phys. Rev. Lett. 118 146601 Google Scholar
[23]	Ren W, Geng H, Zhang Z, Zhang L 2017 Phys. Rev. Lett. 118 245901 Google Scholar
[24]	He J, Amsler M, Xia Y, Naghavi S S, Hegde V I, Hao S, Goedecker S, Ozolins V, Wolverton C 2016 Phys. Rev. Lett. 117 046602 Google Scholar
[25]	Cao Y, Su X, Meng F, Bailey T P, Zhao J, Xie H, He J, Uher C, Tang X 2020 Adv. Funct. Mater. 30 2005861 Google Scholar
[26]	Su X, Zhao N, Hao S, Stoumpos C C, Liu M, Chen H, Xie H, Zhang Q, Wolverton C, Tang X, Kanatzidis M G 2018 Adv. Funct. Mater. 29 1806534 Google Scholar
[27]	Shen X, Wang G, Li S, Yang C C, Tan H, Zhang Y, Lu X, He J, Wang G, Zhou X 2019 J. Alloy. Compd. 805 444 Google Scholar
[28]	Shen X, Shaheen N, Zhang A, Yang D, Yao W, Wang G, Lu X, Zhou X 2017 RSC Advances 7 12719 Google Scholar
[29]	Panda R, Naik R, Mishra N C 2019 J. Alloy. Compd. 778 819 Google Scholar
[30]	Shen X, Zhang B, Chen Q, Tan H, Zhang X, Wang G, Lu X, Zhou X 2019 Inorg. Chem. Front. 6 3545 Google Scholar
[31]	Ying P Z, Zhou H, Gao Y L, Li Y Y, Li Y P, Lian X L, Cui J L 2012 Key Eng. Mater. 519 188 Google Scholar
[32]	Xie H, Hao S, Cai S, Bailey T P, Uher C, Wolverton C, Dravid V P, Kanatzidis M G 2020 Energy Environ. Sci. 13 3693 Google Scholar
[33]	Xie H, Hao S, Bailey T P, Cai S, Zhang Y, Slade T J, Snyder G J, Dravid V P, Uher C, Wolverton C, Kanatzidis M G 2021 J. Am. Chem. Soc. 143 5978 Google Scholar
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Vol. 71, Issue 11 - 2022-06-05

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Structure and thermoelectric performance of Ag_yIn_3.33–y/3Se₅ compounds