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Achieving sustainable zero-waste and carbon neutral solutions that contribute to a circular economy is critically important for the long-term prosperity and continuity of traditional carbon-based energy industries. The Estonian oil shale (OS) sector is an example where such solutions are more than welcome. The combustion of OS generates a continuous flow of ashes destined to landfills. In this study, the technical feasibility of producing monolith building materials incorporating different OS ashes from Estonia was evaluated. Three binder systems were studied: self-cementation of the ashes, ceramic sintering in clay brick production and accelerated carbonation of OS ash (OSA) compacts. Results showed that most of the OSAs studied have low self-cementitious properties and these properties were affected by ash fineness and mineralogical composition. In case of clay bricks, OSA addition resulted in a higher porosity and improved insulation properties. The carbonated OSA compacts showed promising compressive strength. Accelerated carbonation of compacted samples was found to be the most promising way for the future utilization of OSAs as sustainable zero-waste and carbon neutral solution.

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Summary Oxy‐fuel (OF) combustion is considered as one of the promising carbon capture and storage technologies for reducing CO2 emissions from power plants. In the current work, the thermal behaviour of Estonian oil shale (EOS) and its semicoke (SC), pine saw dust, and their blends were studied comparatively under model air (21%O2/79%Ar) and OF (30%O2/70%CO2) conditions using thermogravimetric analysis. Mass spectrometry analysis was applied to monitor the evolved gases. The effect of SC and pine saw dust addition on different combustion stages was analysed using kinetic analysis methods. In addition, different co‐firing cases were simulated using the ASPEN PLUS V8.6 (APV86) software tool to evaluate the effects of blending EOS with different biomass fuels of low and high moisture contents. The specific boiler temperatures of each simulated case with the same adjusted thermal fuel input were calculated while applying the operation conditions of air and OF combustion. According to the experiment and process simulation results, the low heating value and high carbonate content of SC brings along endothermic decomposition of carbonates, which negatively affects the heat balance during the conventional co‐combustion of EOS with SC. Instead, firing of EOS with SC and biomass in OF process can be an effective solution to reduce the environmental impact in terms of the reduction of CO2 emissions and ash. Furthermore, the sensible heat from SC can positively affect the energy balance of the system as the endothermic effect of decomposition of CaCO3 (for both EOS and SC) can be avoided in OF combustion.

In this study, fly ash (FA) compacts were prepared by accelerated carbonation as a potential sustainable building material application with the locally available ashes (oil shale ash (OSA), wood ash (WA) and land filled oil shale ash (LFA)) of Estonia. The carbonation behaviour of FAs and the performance of 100% FA based compacts were evaluated based on the obtained values of CO2 uptake and compressive strength. The influence of different variables (compaction pressure, curing temperature, CO2 concentration, and pressure) on the CO2 uptake and strength development of FA compacts were investigated and the reaction kinetics of the carbonation process were tested by different reaction-order models. A reasonable relation was noted between the CO2 uptake and compressive strength of the compacts. The porous surface structure of the hydrated OSA and WA compacts was changed after carbonation due to the calcite formations (being the primary carbonation product), especially on portlandite crystals. The increase of temperature, gas pressure, and CO2 concentration improved the CO2 uptake levels of compacts. However, the positive effect of increasing compaction pressure was more apparent on the final strength of the compacts. The obtained compressive strength and CO2 uptake values of FA compacts were between 10 and 36 MPa and 11 and 13 wt%, respectively, under various operation conditions. Moreover, compacts with mixed design (OSA/LFA and WA/LFA) resulted in low-strength and density compared to the single behaviour of OSA and WA compacts, yet a higher CO2 uptake was achieved (approximately 15% mass) with mixed design. The conformity of Jander equation (3D-diffusion-limited reaction model) was higher compared to other tested reaction order models for the representation of the carbonation reaction mechanism of OSA and WA. The activation energy for OSA compact was calculated as 3.55 kJ/mol and for WA as 17.06 kJ/mol.