Summary: | Cement production is currently the largest single industrial emitter of CO₂, accounting for∼8% (2.8 Gtons/y) of global CO₂ emissions.Deep decarbonization of cement manufacturing will require remediation of both the CO₂ emissions due to the decomposition of CaCO₃ to CaO and that due to combustion of fossil fuels (primarily coal) in calcining (∼900 °C) and sintering (∼1,450 °C). Here, we demonstrate an electrochemical process that uses neutral water electrolysis to produce a pH gradient in which CaCO₃is decarbonated at low pH and Ca(OH)₂ is precipitated at high pH, concurrently producing a high-purity O₂/CO₂ gas mixture (1:2 molarratio at stoichiometric operation) at the anode and H₂ at the cathode. We show that the solid Ca(OH)₂ product readily decomposes and reacts with SiO₂ to form alite, the majority cementitious phasein Portland cement. Electrochemical calcination produces concentrated gas streams from which CO₂ may be readily separated and sequestered, H₂ and/or O₂ may be used to generate electric power via fuel cells or combustors, O₂ may be used as a component ofoxyfuel in the cement kiln to improve efficiency and lower CO₂ emissions, or the output gases may be used for other value-added processes such as liquid fuel production. Analysis shows that if the hydrogen produced by the reactor were combusted to heat the high-temperature kiln, the electrochemical cement process could be powered solely by renewable electricity.
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