Joining of Co coated ferritic stainless steel to ceramic solid oxide cells by a novel Ag-SiO2 braze

doi:10.1016/j.jmst.2022.01.009

Abstract

Abstract:

A novel Ag-SiO₂ braze for Solid Oxide Cells was successfully developed and applied to join Co coated AISI 441 ferritic stainless steel to YSZ-NiO half cells. The braze showed an improved wettability on the coated steel and the YSZ compared to pure Ag. A defect-free steel/YSZ joint was obtained using an Ag-1SiO₂ braze jointed at 1000 °C for 30 min in air. The microstructure of the joints was characterized by scanning electron microscopy and transmission electron microscopy with energy-dispersive X-ray spectroscopy. Furthermore, a Co-Si-O₂ phase diagram was calculated and used to explain the experimental results and formulate a reaction mechanism. It was found, that during the air brazing process, Co₃O₄ and (Co, Fe)₃O₄ are formed by the oxidation of the prefabricated Co coating. The growth of Cr₂O₃ was effectively impeded by the formed Co-based spinels. In a second step, Co₃O₄ reacts with the SiO₂ present in braze. The Co₂SiO₄ formed by the reaction ensures a firm bonding between the steel and Ag-SiO₂ braze.

Key words: Co coated stainless steel, YSZ-NiO half cell, Microstructure, Interfacial reaction, Joining, Ag-SiO₂ braze, Solid Oxide Cells

Zhiquan Wang, Chun Li, Ragnar Kiebach, Ilaria Ritucci, Ming Chen, Jian Cao. Joining of Co coated ferritic stainless steel to ceramic solid oxide cells by a novel Ag-SiO₂ braze[J]. J. Mater. Sci. Technol., 2022, 121: 174-180.

Figures/Tables 12

Table 1. Chemical composition of AISI 441 ferritic stainless steel used in this study (wt.%).

Alloy	Fe	Cr	Mn	Ni	Ti	Nb	C	Si	S	P
441	Bal.	17.8	0.2	0.18	0.17	0.01	0.01	0.02	0.01	0.01

Table 2. Composition of brazes used in this study (wt.%).

Composition	Ag	Ag-0.5SiO₂	Ag-1SiO₂
SiO₂	0	0.5	1
Ag	100	99.5	99

Fig. 1. Wetting angles of the Ag-SiO2 braze with different composition on YSZ and Co coated steels: (a) Ag/YSZ; (b) Ag-0.5SiO2/YSZ; (c) Ag-1SiO2/YSZ; (d) Ag/coated steel; (e) Ag-0.5SiO2/coated steel; (f) Ag-1SiO2/coated steel.

Fig. 2. (a) Cross-sectional microstructure of Co coated steel/YSZ-NiO half cell joints brazed using Ag-1SiO2; Magnified images of the (b) interface I and (c) interface II marked in Fig. 2(a).

Table 3. Chemical composition of points marked in Fig. 2 (at.%).

Points	Fe	Cr	Co	Ag	Si	O	Zr	Possible phase
A	77.6	17.0	5.4	-	-	-	-	Fe-Cr
B	9.9	48.3	3.9	-	-	37.9	-	Cr₂O₃
C	10.3	1.1	32.6	-	-	56.0	-	(Co, Fe)₃O₄
D	2.5	0.6	54.7	-	-	42.2	-	Co₃O₄
E	2.8	-	37.8	-	15.4	44.0	-	Co₂SiO₄
F	-	-	-	9.4	23.8	66.8	-	SiO₂
G	-	-	-	94.3	3.6	2.1	-	Ag
H	-	-	-	-	-	37.3	62.7	ZrO₂

Fig. 3. (a) BSE image and elemental distribution of coated steel/YSZ-NiO half cell joints achieved by Ag-1SiO2 braze: (b) Fe; (c) Cr; (d) Co; (e) Si; (f) O; (g) Ag; (h) Ni.

Fig. 4. TEM bright-field image of the braze/steel interface and the corresponding EDS line scanning analysis results.

Fig. 5. SAED patterns of (a) Ag, (b) Co2SiO4, and (c) Co3O4; HRTEM of (d) Ag, (e) Co2SiO4, and (f) Co3O4.

Fig. 6. (a) HAADF image of Ag/Co2SiO4 interface with the element distribution of (b) Ag, (c) Co, (d) Si, and (e) O detected by EDS in STEM mode.

Fig. 7. (a) HAADF image of Co2SiO4/ Co3O4 interface with the element distribution of (b) Co, (c) Si, and (d) O detected by EDS in STEM mode.

Fig. 8. Calculated Co-Si-O2 phase diagram.

Fig. 9. Schematic diagrams of microstructure evolution of the Co coated steel/Ag-SiO2 braze interface: (a) joining assembly; (b) the heating process; (c) the melting of braze and interfacial reaction; (d) the final microstructure of the interface.

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Joining of Co coated ferritic stainless steel to ceramic solid oxide cells by a novel Ag-SiO₂ braze

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