The widespread deployment of limestone calcined clay cement (LC3) is constrained by its dependence on high-grade kaolinitic clays. Abundant, low-grade clays often exhibit poor pozzolanic reactivity and require tailored activation strategies. This study proposes a novel clay activation approach using oxalic acid, an organic acid producible through electrochemical CO2 reduction utilizing a waste carbon stream, for the development of LC3. Three activation regimes were examined: thermal activation (TH), thermal followed by oxalic acid immersion (TI), and co-calcination with oxalic acid (CT). Comprehensive characterization (XRF, QXRD, R3) reveals that the CT method uniquely enhances reactivity by promoting selective leaching of Fe2O3 and enriching Al2O3 content, while also inducing mineralogical transitions from quartz to more reactive phases like cristobalite. The R3 test confirmed CT’s superiority, showing the highest bound water content (14.4 %) and showed a significant correlation with strength at all ages (correlation co-efficient ranging from 0.89 to 0.94). In LC3 binders, CT-activated clay yielded a more balanced hydration phase assemblage, accelerating early-age hydration. This translated directly to superior mechanical performance; LC3-CT blends nearly met the ASTM strength criterion (i.e., 42.5 MPa) benchmark at 28 days (within 1 % deviation), significantly outperforming LC3-TH blends (10 % deficit). Despite the added acid, the LC3-CT system maintains a compelling environmental advantage, achieving 21–23 % reductions in CO2 emissions compared to OPC, alongside cost savings of 8–11 %. Results establish CT activation as a technically superior and environmentally sustainable pathway for valorizing low-grade clays. By simultaneously enhancing reactivity and leveraging CO2 utilization, this approach strengthens the foundation for next-generation, low-carbon cement technologies.
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