Metals and alloys are among the most technologically important materials for our industrialized societies. They are the most common structural materials used in cars, airplanes and buildings, and constitute the technological core of most electronic devices. They allow the transportation of energy over great distances and are exploited in critical parts of renewable energy technologies. Even though primary metal production industries are mature and operate optimized pyrometallurgical processes, they extensively rely on cheap and abundant carbonaceous reactants (fossil fuels, coke), require high power heating units (which are also typically powered by fossil fuels) to calcine, roast, smelt and refine, and they generate many output streams with high residual energy content. Many unit operations also generate hazardous gaseous species on top of large CO₂ emissions which require gas-scrubbing and capture strategies for the future. Therefore, there are still many opportunities to lower the environmental footprint of key pyrometallurgical operations. This paper explores the possibility to use greener reactants such as bio-fuels, bio-char, hydrogen and ammonia in different pyrometallurgical units. It also identifies all recycled streams that are available (such as steel and aluminum scraps, electronic waste and Li-ion batteries) as well as the technological challenges associated with their integration in primary metal processes. A complete discussion about the alternatives to carbon-based reduction is constructed around the use of hydrogen, metallo-reduction as well as inert anode electrometallurgy. The review work is completed with an overview of the different approaches to use renewable energies and valorize residual heat in pyrometallurgical units. Finally, strategies to mitigate environmental impacts of pyrometallurgical operations such as CO₂ capture utilization and storage as well as gas scrubbing technologies are detailed. This original review paper brings together for the first time all potential strategies and efforts that could be deployed in the future to decrease the environmental footprint of the pyrometallurgical industry. It is primarily intended to favour collaborative work and establish synergies between academia, the pyrometallurgical industry, decision-makers and equipment providers. Graphical Highlights: A more sustainable production of metals using greener reactants, green electricity or carbon capture is possible and sometimes already underway. More investments and pressure are required to hasten change. Discussion: Is there enough pressure on the aluminum and steel industries to meet the set climate targets? The greenhouse gas emissions of existing facilities can often be partly mitigated by retrofitting them with green technologies, should we close plants prematurely to build new plants using greener technologies? Since green or renewable resources presently have limited availability, in which sector should we use them to maximize their benefits?

Review of principles and limitations of viscosity models for ionic liquids and their mixtures focusing on the use of inappropriate mixing rules for molten salts.

Heat-treatment of spodumene concentrate at 1323 K (1050 °C) for 30 min in a rotary kiln yielded a successful decrepitation. Particle size decreased from 2 cm to less than 425 µm for 80% of the initial mass. X-ray analysis of both fractions did not reveal the presence of α-spodumene or γ-spodumene. The coarse fraction was ground to less than 425 µm with minimal mechanical energy and mixed with the finer fraction to perform lithium extraction. The lithium extraction efficiency reached 98 wt% without the need for flotation. Some aspects of the thermodynamic behavior of the spodumene system were assessed. Results show that metastable γ-spodumene may hinder the formation of β-spodumene at lower heat treatment temperatures. Some heat-treated samples presented non-negligible γ-spodumene content and lithium extraction efficiency decreases as the γ content increases. Finally, the assumed irreversibility of the transformations was studied by analyzing heat-treated samples following long controlled-storage periods. The results show that concentrate composition is not static over the studied time. This suggests that the β formation is not as irreversible as claimed. It is recommended to avoid long periods between heat-treatment and extraction to avoid the slow conversion of β-spodumene to other allotropes, which are less susceptible to lithium extraction.

The discovery of new metallic materials is of prime importance for the development of new technologies in many fields such as electronics, aerial and ground transportation as well as construction. These materials require metals which are obtained from various pyrometallurgical processes. Moreover, these materials need to be synthesized under extreme conditions of temperature where liquid solutions are produced and need to be contained. The design and optimization of all these pyrometallurgical processes is a key factor in this development. We present several examples in which computational thermochemistry is used to simulate complex pyrometallurgical processes including the Hall–Heroult process (Al production), the PTVI process (Ni production), and the steel deoxidation from an overall mass balance and energy balance perspective. We also show how computational thermochemistry can assist in the material selection in these extreme operation conditions to select refractory materials in contact with metallic melts. The FactSage thermochemical software and its specialized databases are used to perform these simulations which are proven here to match available data found in the literature.

The design of multicomponent alloys used in different applications based on specific thermo-physical properties determined experimentally or predicted from theoretical calculations is of major importance in many engineering applications. A procedure based on Monte Carlo simulations (MCS) and the thermodynamic integration (TI) method to improve the quality of the predicted thermodynamic properties calculated from classical thermodynamic calculations is presented in this study. The Gibbs energy function of the liquid phase of the Cu–Zr system at 1800 K has been determined based on this approach. The internal structure of Cu–Zr melts and amorphous alloys at different temperatures, as well as other physical properties were also obtained from MCS in which the phase trajectory was modeled by the modified embedded atom model formalism. A rigorous comparison between available experimental data and simulated thermo-physical properties obtained from our MCS is presented in this work. The modified quasichemical model in the pair approximation was parameterized using the internal structure data obtained from our MCS and the precise Gibbs energy function calculated at 1800 K from the TI method. The predicted activity of copper in Cu–Zr melts at 1499 K obtained from our thermodynamic optimization was corroborated by experimental data found in the literature. The validity of the amplitude of the entropy of mixing obtained from the in silico procedure presented in this work was analyzed based on the thermodynamic description of hard sphere mixtures.