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Towards Electrochemical Synthesis of Cement — an Electrolyzer-Based Process for Decarbonating CaCO 3 while Producing Useful Gas Streams

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Abstract

Cement production is currently the largest single industrial emitter of CO 2 , accounting for 8% (2.8 Gtons/year) of global CO 2 emissions in 2015. Deep decarbonization of cement manufacturing will require remediation of both the CO 2 emissions due to the decomposition of CaCO 3 to CaO, and that due to combustion of fossil fuels (primarily coal) in the calcining (~900°C) and sintering (~1,450°C) processes. Here, we demonstrate an electrochemical process that uses neutral water electrolysis to produce a pH gradient in which CaCO 3 is decarbonated at low pH and Ca(OH) 2 is precipitated at neutral to high pH, concurrently producing a high purity O 2 /CO 2 gas mixture (1:2 molar ratio at demonstrated stoichiometric operation) at the anode and H 2 at the cathode, as shown in Figure 1. We show that the solid Ca(OH) 2 product readily decomposes and reacts with SiO 2 to form alite, the majority cementitious phase in Portland cement. Our electrochemical calcination approach produces concentrated gas streams from which the CO 2 may be readily separated and sequestered, the H 2 and/or O 2 may be used to generate electric power via fuel cells or combustors, the O 2 may be used as a component of oxyfuel in the cement kiln to further lower CO 2 and NO x emissions, or the output gases may be used for other value-added processes including liquid fuel production. Analysis shows that in a scenario where the hydrogen produced by the reactor is combusted to heat the high temperature kiln, the electrochemical cement process can be powered solely by renewable electricity. Figure 1. Schematic of the electrolyzer-based decarbonation cell. Reactions 1a and 1b are the O 2 evolution and H 2 evolution half-cell reactions respectively, under near-neutral pH. Reactions 2a and 2b represent the decomposition of CaCO 3 and release of CO 2 . Reaction 3 is the normal formation of water from its component ions. In Reaction 4, the hydroxide ions in Reaction 3 instead go towards the formation of Ca(OH) 2 , and the protons protonate carbonate ions (Reaction 2b). The overall reaction in which CaCO 3 is converted to Ca(OH) 2 with the attendant release of H 2 , O 2 and CO 2 is shown at the bottom. Figure 1

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... Over the past few decades, there has been a growing interest in optimising the environmental impact of structures to cope with global circumstances and urge governmental and constitutional obligations. On the one hand, researchers have been looking into cutting the carbon emissions associated with material production as steel and cement manufacturing account for 4% and 8% of global carbon emissions respectively [6][7][8]. This resulted in a wide body of research addressing producing cleaner steel from recycled content and less emitting manufacturing techniques [9][10][11] as well as developing innovative non-cementitious binders [12][13][14][15]. ...
... Accordingly, the friction coefficient can be calculated as shown in Eqs. (5)(6)(7)(8). ...
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