High-temperature dolomite decomposition: An integrated experimental and computational fluid dynamics analysis for calcium looping and industrial applications

•Investigated thermal decomposition at high temperatures of dolomite for CaL.•TGA and CFD were used to study reaction kinetics and transport phenomena.•Experimentally validated CFD model revealed fluid-particle interactions.•Findings show dolomite porosity decreases with higher temperature and reaction time.•Effective thermal conductivity increases with calcination temperature and porosity. The thermal decomposition of dolomite was investigated as a potential low-cost and high-performance precursor to CaO in the calcium looping process, which shows great promise when integrated with carbon capture and storage and thermochemical energy storage technologies. Experimental thermogravimetric analysis (TGA) and computational fluid dynamics (CFD) modelling were used to study the isothermal calcination process of dolomite considering industrially relevant conditions, focusing on high temperatures (800–1200 °C), sample sizes (12–18 mm), different calcination atmospheres (air and CO2) and gas velocities (0.2–3 m·s−1). Based on experimental findings, optimal calcination conditions for industrial applications require a minimum temperature of 1000 °C to achieve complete conversion within 25 min and smaller particles for faster conversion rates. Calcination atmosphere is flexible as CO2 concentration shows minimal impact on conversion rates. Laminar flow gas velocity is not a limiting factor and its value should be considered based on other aspects (i.e., costs). Higher particle initial porosity is seen to increase reactivity and thermal efficiency. The CFD model was validated with experimental data, resulting in determination coefficients (R2) higher than 0.9 for all simulated cases. Model predictions revealed insights into particle level phenomena during calcination, such as increased rates at higher temperatures with proportional self-cooling effects, wake formation enhancing fluid mixing and the presence of a thermal boundary layer reducing heat transfer. The findings presented in this paper can be used in future work to determine reaction mechanisms and optimize kinetic parameters for decomposition, as well as further optimize other aspects of the process at industrially relevant operating conditions.