Impact of Si on the high-temperature oxidation of AlCr(Si)N coatings

doi:10.1016/j.jmst.2021.04.065

Abstract

Abstract:

The resistance of wear protective coatings against oxidation is crucial for their use at high temperatures. Here, three nanocomposite AlCr(Si)N coatings with a fixed Al/Cr atomic ratio of 70/30 and a varying Si-content of 0 at.%, 2.5 at.% and 5 at.% were analyzed by differential scanning calorimetry, thermogravimetric analysis and X-ray in order to understand the oxidation behavior depending on their Si-content. Additionally, a partially oxidized AlCrSiN coating with 5 at.% Si on a sapphire substrate was studied across the coating thickness by depth-resolved cross-sectional X-ray nanodiffraction and scanning trans-mission electron microscopy to investigate the elemental composition, morphology, phases and residual stress evolution of the oxide scale and the non-oxidized coating underneath. The results reveal enhanced oxidation properties of the AlCr(Si)N coatings with increasing Si-content, as demonstrated by a retarded onset of oxidation to higher temperatures from 1100°C for AlCrN to 1260°C for the Si-containing coatings and a simultaneous deceleration of the oxidation process. After annealing of the AlCrSiN sample with 5 at.% Si at an extraordinary high temperature of 1400°C for 60 min in ambient air, three zones developed throughout the coating strongly differing in their composition and structure: (i) a dense oxide layer comprising an Al-rich and a Cr-rich zone formed at the very top, followed by (ii) a fine-grained transition zone with incomplete oxidation and (iii) a non-oxidized zone with a porous structure. The varying elemental composition of these zones is furthermore accompanied by micro-structural variations and a complex residual stress development revealed by cross-sectional X-ray nanodiffraction. The results provide a deeper understanding of the oxidation behavior of AlCr(Si)N coatings depending on their Si-content and the associated elemental, microstructural and residual stress evolution during high-temperature oxidation.

Key words: AlCrSiN, Nanocomposite, Cathodic arc, Oxidation behaviour, Cross-sectional X-ray nanodiffraction

Nikolaus Jäger, Michael Meindlhumer, Michal Zitek, Stefan Spor, Hynek Hruby, Farwah Nahif, Jaakko Julin, Martin Rosenthal, Jozef Keckes, Christian Mitterer, Rostislav Daniel. Impact of Si on the high-temperature oxidation of AlCr(Si)N coatings[J]. J. Mater. Sci. Technol., 2022, 100: 91-100.

Figures/Tables 7

Table 1 Elemental composition of the coatings obtained by ERDA.

Cathode composition	Coating composition [at.%/wt.%]
	Al	Cr	Si	N	Al/Cr
Al₇₀Cr₃₀	32.6/35.7	16.7/35.3	0	51.0/29.0	2.0/1
Al_66.5Cr_28.5Si₅	32.6/36.8	14.0/30.5	2.6/3.1	50.6/29.7	2.3/1.2
Al₆₃Cr₂₇Si₁₀	30.8/34.9	13.7/29.9	4.7/5.5	50.5/29.7	2.2/1.2

Fig. 1. SEM fracture cross-section images of (a) AlCrN, (b) AlCrSi2.5N and (c) AlCrSi5N coatings on a WC-Co substrates.

Fig. 2. (a) DSC and (b) TG curves of AlCrN, AlCrSi2.5N and AlCrSi5N coating powders in synthetic air. Annealing temperatures for ex-situ XRD measurements of powders are given.

Fig. 3. X-ray diffractograms of (a) AlCrN, (b) AlCrSi2.5N and (c) AlCrSi5N coatings in the as-deposited state and after annealing at various temperatures in ambient air. Diffractograms with extended 2 angle are given in the supplementary Figure A.2 showing more details about the oxides formed in the Si-containing coatings after the DSC/TG experiment at 1460°C.

Fig. 4. Evolution of phases of AlCrN, AlCrSi2.5N and AlCrSi5N coatings as a function of temperature.

Figure 5. (a) SEM micrograph of the partially oxidized AlCrSi5N sample on a sapphire substrate (with included EDX line-scans), (b) phase evolution, (c) the residual stress development and (d) the FWHM values as a function of coating depth.

Fig. 6. STEM micrographs of the partially oxidized AlCrSi5N coating showing (a) an overview across the coating thickness as imaged by HAADF and EDX maps of (b) the oxide layer, (c) the transition zone and (d) the non-oxidized coating.

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