Interface Stability of Skutterudite Thermoelectric Materials/Ti88Al12

doi:10.15541/jim20170517

Abstract

Abstract:

Interface stability is one of the key issues determining the service reliability and life of thermoelectric devices. For skutterudite-based thermoelectric devices, the barrier layer is required in order to restrain the inter-diffusion between the hot-side electrode and skutterudite matrix. In this work, Ti₈₈Al₁₂was selected as the barrier layer. N-type Yb_0.3Co₄Sb₁₂/Ti₈₈Al₁₂/Yb_0.3Co₄Sb₁₂ and p-type CeFe_3.85Mn_0.15Sb₁₂/Ti₈₈Al₁₂/CeFe_3.85Mn_0.15Sb₁₂thermoelectric joints were prepared by one-step hot pressing sintering method. The evolution processes of contact resistivity and microstructure were studied through accelerated aging experiments. The results show that the contact resistivity of n-type joints increases slower than that of p-type joints under the same aging condition. Activation energy for n-type and p-type joints is 84.1 kJ/mol and 68.8 kJ/mol, respectively. Growth of the inter-metallic compound layer and cracking at the AlCo/TiCoSb interface result in rapidly increased contact resistivity of n-type joints. For p-type joints, the difference of coefficient of thermal expansion between CeFe_3.85Mn_0.15Sb₁₂ and Ti₈₈Al₁₂ becomes the main reason for the cracks.

Key words: skutterudite, interface stability, barrier layer, contact resistivity

CLC Number:

TQ174

ZHANG Qi-Hao, LIAO Jin-Cheng, TANG Yun-Shan, GU Ming, LIU Rui-Heng, BAI Sheng-Qiang, CHEN Li-Dong. Interface Stability of Skutterudite Thermoelectric Materials/Ti₈₈Al₁₂[J]. Journal of Inorganic Materials, 2018, 33(8): 889-894.

Figures/Tables 9

Fig. 1 Variation of specific contact resistivity (ρc) with thermal aging time and temperature: (a) n-type Yb0.3Co4Sb12/Ti88Al12/Yb0.3Co4Sb12; (b) p-type CeFe3.85Mn0.15Sb12/Ti88Al12/CeFe3.85Mn0.15Sb12; Variation of lnk with 1000/T: (c) n-type; (d) p-type

Fig. 2 As-prepared n-type Yb0.3Co4Sb12/Ti88Al12/Yb0.3Co4Sb12 interface (a) SEM image; EDS mapping results of (b) Co; (c) Sb; (d) Ti; (e) Al and (f) EDS point analysis location

Table 1 EDS point analysis results

Point	Co/at%	Sb/at%	Ti/at%	Al/at%
1	0	36.74	63.26	0
2	0	59.19	33.87	6.94
3	30.11	31.01	33.23	5.65
4	48.04	0.49	3.75	47.72
5	0	56.36	33.14	10.50
6	0	66.92	33.08	0

Fig. 3 SEM images of n-type Yb0.3Co4Sb12/Ti88Al12/Yb0.3Co4Sb12 interface after thermal aging at 550℃ for different days(a) 0 d; (b) 8 d; (c) 18 d; (d) 38 d

Fig. 4 SEM images of n-type Yb0.3Co4Sb12/Ti88Al12/Yb0.3Co4Sb12 interface after thermal aging(a) 550℃, 38 d; (b) 575℃, 38 d; (c) 600℃, 38 d

Fig. 5 As-prepared p-type CeFe3.85Mn0.15Sb12/Ti88Al12/ CeFe3.85Mn0.15Sb12 interface (a) SEM image; EDS mapping results of (b) Ti; (c) Al; (d) Fe; (e) Sb; (f) Mn; (g) EDS line scanning location, and (h) the corresponding result

Fig. 6 SEM images of p-type CeFe3.85Mn0.15Sb12/Ti88Al12/CeFe3.85Mn0.15Sb12 interface after thermal aging at 550℃ for different days(a) 0 d; (b) 2 d and (c) the corresponding EDS mapping result; (d) 12 d and (e) the corresponding EDS mapping result; (f) 38 d

Fig. 7 SEM images of p-type CeFe3.85Mn0.15Sb12/Ti88Al12/CeFe3.85Mn0.15Sb12 interface after thermal aging

Fig. 8 The variation of thermal expansion coefficient of different materials as function of the temperature

References 21

[1]	ZHANG Q H, HUANG X Y, BAI S Q,et al. Thermoelectric devices for power generation: recent progress and future challenges.Advanced Engineering Materials, 2016, 18(2): 194-213.
[2]	SHI X, CHEN L, UHER C.Recent advances in high-performance bulk thermoelectric materials.International Materials Reviews, 2016, 6: 1-37.
[3]	FAN J, CHEN L, BAI S,et al. Joining of Mo to CoSb3 by spark plasma sintering by inserting a Ti interlayer.Materials Letters, 2004, 58(30): 3876-3878.
[4]	YANG X Y, WU J H, GU M,et al. Fabrication and contact resistivity of W-Si3N4/TiB2-Si3N4/p-SiGe thermoelectric joints.Ceramics International, 2016, 42(7): 8044-8050.
[5]	LIN Y C, LEE K T, HWANG J D,et al. Solid liquid interdiffusion bonding of Zn4Sb3 thermoelectric material with Cu electrode.Journal of Electronic Materials, 2016, 45(10): 1-8.
[6]	TANG Y S, BAI S Q, REN D D,et al. Interface structure and electrical property of Yb0.3Co4Sb12/Mo-Cu element prepared by welding using Ag-Cu-Zn solder.Journal of Inorganic Materials, 2015, 30(3): 256-260.
[7]	ZHAO D G, WANG L, CAI Y H,et al. One-step sintering of CoSb3 thermoelectric material and Cu-W alloy by spark plasma sintering.Materials Science Forum, 2009, 610: 389-393.
[8]	ZHAO D, LI X, HE L,et al. Interfacial evolution behavior and reliability evaluation of CoSb3/Ti/Mo-Cu thermoelectric joints during accelerated thermal aging.Journal of Alloys & Compounds, 2009, 477(1/2): 425-431.
[9]	GU M, XIA X, LI X,et al. Microstructural evolution of the interfacial layer in the TiAl/Yb0.6Co4Sb12 thermoelectric joints at high temperature.Journal of Alloys & Compounds, 2014, 610: 665-670.
[10]	GU M, XIA X, HUANG X,et al.Study on the interfacial stability of p-type Ti/CeyFexCo4-xSb12 thermoelectric joints at high temperature Journal of Alloys & Compounds, 2016, 671: 238-244.
[11]	SALES B C, MANDRUS D, WILLIAMS R K.Filled skutterudite antimonides: a new class of thermoelectric materials.Science, 1996, 272(5266): 1325-1328.
[12]	SHI X, YANG J, SALVADOR J R,et al. Multiple-filled skutterudites: high thermoelectric figure of merit through separately optimizing electrical and thermal transports.Journal of the American Chemical Society, 2011, 133(20): 7837-7846.
[13]	ROGL G, GRYTSIV A, ROGL P,et al.N-type skutterudites (R, Ba,Yb)yCo4Sb12 (R = Sr, La, Mm, DD, SrMm, SrDD) approaching ZT approximate to 2.0 Acta Materialia, 2014, 63: 30-43.
[14]	EL-GENK M S, SABER H H, CAILLAT T,et al. Tests results and performance comparisons of coated and uncoated skutterudite based segmented unicouples.Energy Conversion & Management, 2006, 47(2): 174-200.
[15]	ZHAO D, LI X, HE L,et al. High temperature reliability evaluation of CoSb3/electrode thermoelectric joints.Intermetallics, 2009, 17(3): 136-141.
[16]	WOJCIECHOWSKI K T, ZYBALA R, MANIA R.High temperature CoSb3-Cu junctions.Microelectronics Reliability, 2011, 51(7): 1198-1202.
[17]	GUO J Q, GENG H Y, OCHI T,et al. Development of skutterudite thermoelectric materials and modules.Journal of Electronic Materials, 2012, 41(6): 1036-1042.
[18]	SONG B, LEE S, CHO S,et al. The effects of diffusion barrier layers on the microstructural and electrical properties in CoSb3 thermoelectric modules.Journal of Alloys & Compounds, 2014, 617(73): 160-162.
[19]	QIU P F, SHI X, LIU R H,et al.Thermoelectric properties of manganese-doped p-type skutterudites CeyFe4-xMnxSb12 Functional Materials Letters, 2013, 6(5): 1340003.
[20]	GU M, BAI S, XIA X,et al. Study on the high temperature interfacial stability of Ti/Mo/Yb0.3Co4Sb12 thermoelectric joints.Applied Sciences, 2017, 7(9): 952.
[21]	张建中. 温差电技术. 天津: 天津科学技术出版社, 2013: 370-371.

Interface Stability of Skutterudite Thermoelectric Materials/Ti₈₈Al₁₂

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