High-efficiency CO₂ sequestration through direct aqueous carbonation of carbide slag: determination of carbonation reaction and optimization of operation parameters

Highlights

● The sequestration capacity of 610.8 g CO₂/kg was achieved for carbide slag.

● Corresponding carbonation efficiency was 62.04% at optimum reaction conditions.

● The mass transfer of CO₂ was the rate-limiting steps at the initial stage.

● The mass transfer of Ca²⁺ controlled the carbonation rate with increasing time.

Abstract

Under the dual-carbon target, CO₂ mineralization through solid wastes presents a mutually beneficial approach for permanent carbon emission reduction at a low material cost, while also enabling the resource utilization of these wastes. However, despite its potential, a comprehensive understanding about the effect of industrial solid waste properties and operating parameters on the carbonation process, and the mechanism of direct aqueous carbonation is still lacking. A series of experiments were conducted to compare the carbonation performance of fly ash, steel slag, and carbide slag. Subsequently, CO₂ mineralization by carbide slag was systematically studied under various operating parameters due to its high CO₂ sequestration capacity. Results showed the reactivity of CaO and Ca(OH)₂ was higher than that of CaO·SiO₂ and 2CaO·SiO₂. Carbide slag demonstrated a sequestration capacity of 610.8 g CO₂/kg and carbonation efficiency ζ_Ca of 62.04% under the conditions of 65 °C, 1.5 MPa initial CO₂ pressure, 15 mL/g liquid-to-solid ratio, and 200 r/min stirring speed. Moreover, the formation of carbonates was confirmed through XRD, SEM-EDS, TG, and FTIR. A mechanism analysis revealed that initially, the rate of the carbonation process was primarily controlled by the mass transfer of CO₂ in the gas–liquid interface. However, the rate-determining step gradually shifted to the mass transfer of Ca²⁺ in the solid–liquid interface as the reaction time increased. This study lays the foundation for the large-scale implementation of CO₂ sequestration through carbide slag carbonation.

Graphical abstract

Keywords

Industrial by-products / Direct aqueous carbonation / CO₂ sequestration / Mass transfer

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Acknowledgements

This work was supported by China Petrochemical Corporation Scientific Research Projects (Nos. 417002-4 and 418020-5).

Conflict of Interest

The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest.

Ethical Approval

This article does not contain any studies with human participants or animals performed by any of the authors.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11783-024-1772-y and is accessible for authorized users.

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