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This study examined the effect of Carbon Capture and Storage units on the environmental, energy and economic performance of the Brazilian electric grid. Four scenarios were established considering the coupling of Calcium Looping (CaL) processes to capture CO2 emitted from thermoelectric using coal and natural gas: S1: the current condition of the Brazilian grid; S2 and S3: Brazilian grid with CaL applied individually to coal (TEC) and gas (TGN) operated thermoelectric; and S4: CaL is simultaneously coupled to both sources. Global warming potential (GWP) expressed the environmental dimension, Primary Energy Demand (PED) was the energy indicator and Levelised Cost of Energy described the economic range. Attributional Life Cycle Assessment for generation of 1.0 MWh was applied in the analysis. None of the scenarios accumulated the best indexes in all dimensions. Regarding GWP, S4 totals the positive effects of using CaL to reduce CO2 from TEC and TGN, but the CH4 emissions increased due to its energy requirements. As for PED, S1 and S2 are similar and presented higher performances than S3 and S4. The price of natural gas compromises the use of CaL in TGN. A combined verification of the three analysis dimensions, proved that S2 was the best option of the series due to the homogeneity of its indices. The installation of CaL in TECs and TGNs was effective to capture and store CO2 emissions, but the costs of this system should be reduced and its energy efficiency still needs to be improved.