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Purpose This work deals with the application of a solidification/stabilization process with the aim to obtain safe and reusable granular materials from a polluted soil and to elucidate the mechanisms involved in the retention of several heavy metals. Materials and methods The High Performance Solidification/Stabilization (HPSS®) process was applied to the selected contaminated soil by using both ordinary Portland cement and calcium aluminate cement, as well as several binders prepared by combining these two types of cement in different proportions. Leaching and mechanical tests were carried out to evaluate the performances of the proposed binders in the pellets produced by the HPSS® process, while XRD analysis and SEM/EDX imaging were used to investigate the phase composition and internal microstructure of the treated samples. Result and discussion The examination of the obtained granular materials revealed that the immobilization of Sb was mainly related to its inclusion within calcium silicate hydrates’ structure; the immobilization of Cr, Pb, Ni, Co, Zn and Tl was associated with the eluate pH and their incorporation within ettringite structure, while for Se, Cu, Ba and V, the main retention mechanism was physical encapsulation. In addition, the application of a wet conditioning process improved the materials’ performance, leading to granules always satisfying the Italian regulatory requirements for reuse. Conclusions The findings obtained in this study were useful to better elucidate the mechanisms involved in the retention of heavy metals by several binders, contributing to the development of sustainable management strategies for contaminated soils and sediments through their transformation into reusable materials. Graphical abstract

The application of an innovative solidification/stabilization (S/S) process was investigated for the remediation of Pb contaminated soil. The performance of Pb stabilization was evaluated by comparing the use of calcium aluminate cement (CAC) and an alkali activated metakaolin binder vs the Ordinary Portland Cement (OPC). The phase composition of the stabilized products was investigated by XRD and correlated to the internal microstructure obtained by SEM-EDX imaging. Leaching tests were performed to ascertain the effectiveness of the proposed binders in the S/S of the contaminated soil, and Pb release was evaluated for each binding system. The overall results proved that multiple mechanisms are involved in Pb retention and that key parameters regulating the stabilization performance are strongly dependent on the type of applied binder system. Pb was found to be associated to C-S-H in the case of OPC, whereas ettringite played a key role in the retention of this contaminant using the CAC binder. The use of a NaOH activated metakaolin resulted in almost total retention of Pb, despite a lack of solidification, highlighting the importance of pH in the regulation of the leaching behavior.

Cement-based stabilization is a widespread technique used for the treatment of contaminated soils. Despite its established application, the mechanisms involved in the stabilization of contaminants are not fully understood yet. This work aims to elucidate the fate of a real Pb contaminated soil amended with different binders, by studying Pb local environment prior and after the stabilization process. The study of a complex historically contaminated soil was coupled with the investigation of simplified artificial systems, developed to model Pb local structure in the unknown newly formed hybrid systems of soil and binders. The use of synchrotron-based element-specific X-ray absorption spectroscopy (XAS) permitted to probe the actual transformation of Pb environment in the real contaminated soil after the stabilization process. With the support of the model systems, we can propose as the main mechanism involved in Pb retention in sulfated soil treated with cement, the incorporation and/or adsorption of Pb on calcium silicate hydrates and ettringite.

Soil and sediment contamination is recognised as one of the most relevant environmental problems caused by past industrial activities and unsustainable waste disposal practices, highlighting the need to develop or improve effective remediation techniques to support sustainable management strategies. In this context, the remediation of sediments dredged from the Mincio river (Italy) contaminated by mercury and heavy hydrocarbons (C12-40) was carried out by applying and implementing the High Performance Solidification/Stabilization technology, aimed at producing safe and reusable cement-based granular materials. The technology was improved by decreasing both the temperature and time of the thermal desorption treatment (from 280 to 110 °C and from 4-16 h to 70 min, respectively) and by including a wet conditioning step to the process. Temperature and time reduction allowed to diminish the degradation of the cementitious phases of the granules (usually related to the high temperatures employed in the process), while the wet conditioning step allowed to improve their mechanical properties, as well as to further reduce the leaching of contaminants. The physical-chemical properties of the granules and contaminant leaching in water were investigated by Inductively Coupled Plasma Mass and Optical Emission Spectrometry, Ultraviolet–Visible spectroscopy, Gas Chromatography, X-Ray Powder Diffraction, and Scanning Electron Microscopy, in order to identify the optimal parameters for both thermal and wet conditioning processes. The overall results showed that the use of consecutive thermal and wet conditioning treatment on sedimentary cementitious materials from the High Performance Solidification/Stabilization technology led to the removal of volatile pollutants and to the improvement of granule quality, thus providing a final material that satisfied all the Italian regulatory requirements for reuse. Therefore, the findings obtained in this study may contribute to the development of sustainable management strategies for contaminated soils and sediments, leading to their valorisation through the transformation into reusable materials.