Halloysite is a clay mineral that has a nanosized tubular morphology and high pozzolanic activity, and its calcination product can be used as a supplementary cementitious material in limestone calcined clay cement (LC3). In this study, the effects of the calcination temperature of halloysite, gypsum content, and water/binder (W/B) ratio on the mechanical properties and microstructures of LC3 were evaluated. The results demonstrated that halloysite calcined at the temperature of 650°C–850°C exhibited high pozzolanic activity: LC3 prepared using halloysite calcined above 650°C exhibited a shorter setting times and higher compressive strengths than those prepared with halloysite calcined at 550°C. This is attributable to the formation of more additional calcium aluminate silicate hydrate gel, and a larger amount of hemicarboaluminate and monocarboaluminate at higher temperatures than at lower temperatures, which results in more filling of pores in LC3 under the former conditions than the later conditions. The results also indicated that the optimum content of additional gypsum for LC3 was between 0 wt% and 2 wt%, and overdose gypsum did not substantially alter their setting times but decrease their compressive strengths. In contrast, a decrease in the W/B ratios decreased their setting times, total porosity, and increased their compressive strengths. Overall, in this study, LC3 prepared using halloysite calcined at 750°C, with a W/B ratio of 0.40 and without additional gypsum, exhibited the highest compressive strengths, which were 42.6, 51.7, and 57.1 MPa after 3, 7, and 28 days of curing, respectively. These findings deepen the research on the hydration mechanism of LC3 prepared with calcined halloysite and provide basic data for the wide application of this approach.
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