This study examines the chemical and mineralogical composition of waste materials from abandoned copper and manganese mines in the Iberian Pyrite Belt, Portugal, as a first step toward their potential recycling for critical and strategic raw materials (CRM and SRM). Using portable X-ray fluorescence (pXRF) and other analytical techniques, this research highlights the presence of valuable elements, including copper, manganese, and rare earth elements, in concentrations significantly above their crustal abundance. The findings underscore the dual potential of these wastes: as sources of secondary raw materials and for mitigating environmental hazards such as acid mine drainage (AMD). Recovered materials include chalcopyrite, pyrolusite, and rhodochrosite, with critical elements like cobalt, lithium, and tungsten identified. pXRF proved to be a reliable, cost-effective tool for rapid field and laboratory analyses, demonstrating high precision and good correlation with standard laboratory methods. The study emphasizes the importance of characterizing historical mining waste to support a circular economy, reduce reliance on foreign material imports, and address environmental challenges. This approach aligns with the European Union’s Critical Raw Materials Act, promoting sustainable resource use and the recovery of strategic resources from historical mining sites.

Mining activity in Algares (Aljustrel Mine, Portuguese sector of the Iberian Pyrite Belt, IPB) stems prior to Roman times. As the orebody is vertical and relatively thin, mining was carried out mainly along underground adits (galleries). Nowadays, the deposit is considered exhausted and the area is being rehabilitated for a different use. The Algares +30 level adit intersects two volcanic units of the IPB Volcano-Sedimentary Complex. The massive sulphide and related stockwork zone are hosted by the Mine Tuff volcanic unit and are exposed in the walls of the gallery, showing intense hydrothermal alteration. Along the mine adit, the geological sequence is affected by strong oxidation and supergene alteration, giving rise to the formation of secondary minerals through the oxidation of the sulphides. The most common minerals found were melanterite (FeSO₄·7H₂O) and chalcanthite (CuSO₄·5H₂O), forming essentially massive or crystalline aggregates, ranging from greenish to bluish colours. Melanterite from the walls revealed to be Cu-rich by opposition to that from stalactites/stalagmites formed below the old ore storage silo revealing the low-copper-grade ores exploited underground. The mineralogy of the efflorescent salts was used to ascertain the processes involved in their formation, and moreover, the inventory of minerals is presented, as well as their principal characteristics.

A steady supply of mineral raw materials is vital for the transition to a low-carbon, circular economy. The number of active mines in Europe has severely declined over the last century and half, giving rise to many abandoned mining waste sites and corresponding geological heritage. Also, the rise in minerals demand for large-scale deployment of renewable energy requires the continued and steady availability of key minerals. The supply risk associated with unpredicted geopolitical events needs to be eliminated/mitigated. Historical mine waste sites are the answer but evaluating mine waste is a lengthy and costly exercise. The study, undertaken in the Lousal Mine, used small unmanned aerial systems (sUASs) to model and determine mine waste volumes by generating orthomosaic maps with quick, inexpensive, and reliable results. Calculated mine waste volumes between 308,478 m³ and 322,455 m³ were obtained. XRD and p-XRF techniques determined the mineralogy and chemistry of waste, which varied from mineralization and host rocks with hydrothermal alteration and numerous neogenic sulphates (mostly gypsum, rhomboclase, ferricopiapite, coquimbite, and jarosite) related with supergene processes and weathering. The study shows the viability of using these sUASs to successfully model historical mine waste sites in an initial phase and for future monitoring programs.

The sheltered environment of the Algares +30 level adit (underground mine gallery) contributes to the preservation of secondary water-soluble minerals formed on the tunnel walls. The massive sulphide and related stockwork zone are hosted by the Mine Tuff volcanic unit and are exposed in the walls of the gallery, showing intense oxidation and hydrothermal alteration. Minerals from the halotrichite group were identified on the efflorescent salts, typically white fine-acicular crystals but also on aggregates with dark orange/brownish colour. Mineral characterization was performed using several methods and analytical techniques (XRD, XRF-WDS, SEM-EDS, DTA-TG), and the chemical formulas were calculated maintaining the ratio A:B ≅ 1:2 in accordance with the general formula of the halotrichite group, AB₂(SO₄)₄·22H₂O. This methodology allowed the assignment of the orange colour to the presence of trivalent iron on iron-rich pickeringite in partial substitution of aluminium.

Abandoned mining areas provide valuable opportunities to investigate ore-forming processes, supergene mineral transformations, and the geochemical behaviour of metals. In this sense, the old Preguiça mine (Beja, Portugal), exploited for Fe–Zn–Pb, was studied providing new mineralogical and geochemical data aimed at improving the understanding of the secondary mineral assemblages of this deposit. A total of 70 samples collected from three accessible underground levels (first, second and third) and mine waste, complemented by 16 samples from a deeper level (fourth) previously collected, were analysed using X-ray diffraction (XRD), scanning electron microscopy (SEM), and a portable X-ray fluorescence (pXRF) equipment. Mineralogical phases are dominated by a wide range of secondary oxides, carbonates, arsenates, vanadates, silicates, phosphates and sulphates, but remnants of primary sulphides were also found. The following minerals can be emphasised: goethite, hematite, calcite, dolomite, descloizite, willemite, mimetite, cerussite, smithsonite and fraipontite. The presence of massicot in the Preguiça mine, is described for the first time. Bulk geochemical analyses show high concentrations of Fe, Ca, Zn and Pb, consistent with the observed mineralogy. The presence of vanadium- and arsenic-bearing minerals highlights the occurrence of critical raw materials, supporting the importance of reassessing other abandoned mining areas in the context of sustainable resource management and strategic raw-material planning.