Abstract
Electrochemical reactors can reduce the carbon intensity of cement production by using electricity to
convert limestone (CaCO3) into Ca(OH)2, which can then be combined with silica (SiO2) at high
temperatures to produce cement clinker. A key challenge with this method is the deposition of solid
Ca(OH)2 at the reactor membrane leads to unacceptably low energy efficiencies. To address this
challenge, we connected the electrochemical reactor (“cement electrolyser”) to a distinctive chemical
reactor (“calcium reactor”) so that Ca(OH)2 could form there instead, and not within the electrochemical
reactor. In this tandem system, the cement electrolyser generated H+ and OH– in the respective chemical
and cathode compartments. The H+ then reacted with CaCO3 to form Ca2+ ions, which were diverted into
the calcium reactor to react with the OH– to form Ca(OH)2. We fabricated a composite membrane to
selectively block the transport of Ca2+ into the cathode compartment. Charge balance in the cement
reactor was enabled with monovalent ions (e.g., K+) as the positive charge carrier. This orthgonalized ion
management was validated by operando imaging. The tandem reactor enabled the electrolysis process to
operate for 50 hours at 100 mA cm-2 without any voltage increase, which represents a meaningful step
forward for cement clinker precursor production.
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