| Summary: | In recent concrete research, a novel category of coatings has emerged: polymers/nanoparticles blends. The efficacy of such coatings warrants extensive examination across various concrete mixtures, particularly those incorporating high-volume supplementary cementitious materials (SCMs) to mitigate carbon footprints, an industry imperative. This study used three vulnerable concrete mixtures to assess the effectiveness of ethyl silicate and high-molecular-weight methyl methacrylate blended with 2.5% and 5% halloysite and montmorillonite nano-clay. Findings from physical, thermal, and microstructural analyses confirmed vulnerabilities in concretes with a high water-to-binder ratio (0.6) under severe exposure conditions, notably with high SCM content (40% and 60% fly ash and slag, respectively). Neat ethyl silicate or high-molecular-weight methyl methacrylate coatings inadequately protected those concretes against physical salt attacks and salt–frost scaling exposures. However, the incorporation of halloysite nano-clay or montmorillonite nano-clay in these polymers yielded moderate-to-superior concrete protection compared to neat coatings. Ethyl silicate-based nanocomposites provided full protection, achieving up to 100% improvement (no or limited surface scaling) against both exposures, particularly when incorporating halloysite-based nano-clay at a 2.5% dosage by mass. In contrast, high-molecular-weight methyl methacrylate-based nano-clay composites effectively mitigated physical salt attacks but exhibited insufficient protection throughout the entire salt–frost scaling exposure, peeling off at 15 cycles.
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