Novel and durable composite phase change thermal energy storage materials with controllable melting temperature

doi:10.1016/j.jmst.2020.12.071

Abstract

Abstract:

The development of high temperature phase change materials (PCMs) with great comprehensive performance is significant in the future thermal energy storage system. In this study, novel and durable Al-Si/Al₂O₃-AlN composite PCMs with controllable melting temperature were successfully synthesized by using pristine Al powder as raw material and tetraethyl orthosilicate as SiO₂ source. The Al₂O₃ shell and Al-Si alloy were in-situ produced via the substitution reaction between molten Al and SiO₂. Importantly, the crack caused by the incomplete encapsulation of the Al₂O₃ shell could repair itself by the nitridation reaction of internal molten Al and thereby forming a highly dense Al₂O₃-AlN composite shell. The produced dense Al₂O₃-AlN composite shell could significantly improve the thermal cycling stability of composite PCMs, and thus, the thermal storage density decrease of the Al-Si/Al₂O₃-AlN (59.8 J/g to 77.7 J/g) was far less than that of the Al-Si/Al₂O₃ (118.5 J/g) after 3000 thermal cycles. Moreover, the synthesized Al-Si/Al₂O₃-AlN still exhibited a controllable melting temperature (571.5-637.9 ℃), relatively high thermal storage density (105.6-150.7 J/g), great dimensional stability and structural stability after 3000 thermal cycles. Hence, the synthesized Al-Si/Al₂O₃-AlN composite PCMs, as promising preferential thermal energy storage materials, can be stably used in the energy utilization efficiency improvement of various systems for more than 6 years.

Key words: Al-Si, Al₂O₃-AlN, Durable, Controllable melting temperature, Phase change thermal storage material

Haiting Wei, Shuiyuan Yang, Cuiping Wang, Changrui Qiu, Kairui Lin, Jiajia Han, Yong Lu, Xingjun Liu. Novel and durable composite phase change thermal energy storage materials with controllable melting temperature[J]. J. Mater. Sci. Technol., 2021, 86: 11-19.

Figures/Tables 13

Fig. 1. Preparation process of synthesized Al-Si/Al2O3 composite PCMs.

Fig. 2. SEM images of (a, a1) pristine Al, (b, b1) CM-4.5-Ar, (c, c1) CM-4.5-N2 obtained at various magnifications, and element (Al, O, Si, N) mappings of sample CM-4.5-N2.

Table 1 Elemental composition of samples CM-4.5-Ar and CM-4.5-N2.

Element	CM-4.5-Ar (at.%)	CM-4.5-N₂ (at.%)
O	48.09	39.59
Al	47.18	46.88
Si	4.73	2.22
N	-	11.31
Total	100.00	100.00

Fig. 3. (a) SEM image and (b) element Al, (c) element O, (d) element Si, (e) element N mappings of cross-sectional CM-4.5-N2; (f) SEM image of cracked CM-4.5-N2.

Fig. 4. XRD patterns of CM-4.5-Ar, CM-4.0-N2, CM-4.5-N2, and CM-5.0-N2.

Fig. 5. DSC (a) heating and (b) cooling curves of synthesized CM-4.5-Ar, CM-4.0-N2, CM-4.5-N2, and CM-5.0-N2.

Table 2 Thermophysical properties of CM-4.5-Ar, CM-4.0-N2, CM-4.5-N2, and CM-5.0-N2.

Sample	Melting temperature (℃)	Melting latent heat (J/g)	Crystallization temperature (℃)	Crystallization latent heat (J/g)
CM-4.5-Ar	573.2/612.3	255.8	571.2/629.8	-248.9
CM-4.0-N₂	570.6/637.9	228.4	640.7	-221.6
CM-4.5-N₂	571.7/627.8	190.5	628.1	-185.2
CM-5.0-N₂	571.5/610.2	165.4	566.5	-160.3

Table 3 Comparison of thermal storage property between some reported high temperature composite PCMs and the Al-Si/Al2O3-AlN synthesized in this study.

Composite PCMs	Melting temperature (℃)	Melting latent heat (J/g)	References
Al-Si/Al₂O₃-Cu	570	100	[4]
Al-Si/Al₂O₃	577	183	[29]
Al-Si/Al₂O₃	577	201	[30]
Bi/Ag	236‒252	20.1-37.6	[35]
Sn_xZn_1-_x/SiO_x	278‒429	67.41-96.09	[23]
Al-Si/Al₂O₃-AlN	571.5‒637.9	165.4‒228.4	This study

Table 4 Thermal conductivity of samples CM-4.5-Ar, CM-4.0-N2, CM-4.5-N2 and CM-5.0-N2.

Sample	Thermal conductivity (W m^-1 K^-1)
CM-4.5-Ar	2.462 ± 2.351 × 10^-3
CM-4.0-N₂	2.134 ± 1.146 × 10^-3
CM-4.5-N₂	1.723 ± 2.342 × 10^-3
CM-5.0-N₂	1.417 ± 1.216 × 10^-3

Fig. 6. DSC heating curves of (a) CM-4.5-Ar, (b) CM-4.0-N2, (c) CM-4.5-N2, and (b) CM-5.0-N2 after 1000, 2000, and 3000 thermal cycles.

Fig. 7. (a) XRD patterns of CM-4.5-N2 after different thermal cycles; SEM images of CM-4.5-N2 after different thermal cycles: (b) 500, (c) 1000, (d) 2000, (e) 3000, and the element mappings of CM-4.5-N2 after 3000 thermal cycles: (f) element Al, (g) element O, (h) element Si, (i) element N.

Fig. 8. Average particle diameter of synthesized CM-4.5-Ar, CM-4.0-N2, CM-4.5-N2, and CM-5.0-N2 before and after 3000 thermal cycles.

Fig. 9. (a) Heating curve of sample CM-4.5-N2 in the calcination process, inset shows the optical images of four intermediate products (S1, S2, S3, S4); (b) XRD patterns of S1, S2, S3, S4, and SEM images of (c) S1, (d) S2, (e) S3, (f) S4.

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