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In this study, we investigate the impact of ageing and high vacuum on existing environmentally friendly Zr4/Cr3-based conversion coatings. The freshly formed coating undergoes several changes during ageing and exposure to high vacuum. Based on the present data, we propose that the coating formed over AA6082 and AA7075 alloys is sol-gel in nature, confirmed by secondary neutral mass spectroscopy (SNMS) using the depth profiling technique. Our findings reveal that there are elemental level changes that result in shrinkage of the coating. Most Zr ions in the coating are in the solute form, with lesser number of Cr and Al ions that disappear under high vacuum over a certain period of time. The remaining Cr, Zr and O atoms exist in a gelatinous state. During ageing, there is a continuous transition of ions from solute to gelatinous state. In addition, the deposition of coating ions is directly influenced by the substrates and their constituents. The extent of dissolution of aluminium in the conversion bath determines both Zr and Cr ion deposition. For a highly alloyed metal like AA7075, the dissolution rate is disturbed by copper and zinc.