| Summary: | The surface properties of two sepiolite samples and one palygorskite sample were compared using inverse gas chromatography (IGC). Samples were previously conditioned at appropriate temperatures for the removal of all zeolitic water. Dispersive (or Lifshitz–van der Waals) component of the surface energy (γ<sub>s</sub><sup>d</sup>), specific interactions (−ΔG<sub>a</sub><sup>s</sup>) with π electron donor bases (1-alkenes), and nanomorphology indices <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msub><mrow><mrow><mo>(</mo><mi>IM</mi><mi mathvariant="sans-serif">χ</mi></mrow></mrow><mi mathvariant="normal">T</mi></msub><mrow><mo>)</mo></mrow></mrow></semantics></math></inline-formula> based on the injections of cycloalkanes and a branched alkane were measured. From IGC data, at 240 °C, it was found that the palygorskite was clearly distinguished from the sepiolites. The palygorskite possessed a lower γ<sub>s</sub><sup>d</sup>, larger −ΔG<sub>a</sub><sup>s</sup> with 1-alkenes, and remarkably higher <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msub><mrow><mrow><mi>IM</mi><mi mathvariant="sans-serif">χ</mi></mrow></mrow><mi mathvariant="normal">T</mi></msub></mrow></semantics></math></inline-formula>. Slight differences could also be observed between the two sepiolite samples with the same origin. The results were rationalized in terms of the structural features of the two studied minerals. The larger channels of the sepiolite allow for a better insertion of the <i>n</i>-alkanes (longer retention times) while excluding the bulkier probes, such as cyclooctane or 2,2,4-trimethylpentane. Accordingly, the corresponding γ<sub>s</sub><sup>d</sup> values were larger and the <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msub><mrow><mrow><mi>IM</mi><mi mathvariant="sans-serif">χ</mi></mrow></mrow><mi mathvariant="normal">T</mi></msub></mrow></semantics></math></inline-formula> values were lower (higher surface nanoroughness) for the sepiolites. Regarding Lewis acid–base properties, all the sample’s surfaces evidenced a very strong amphoteric character. The present results highlight the potential of the evaluated samples for, e.g., adsorption processes with volatile organic compounds or matrix–filler interactions regarding the production of composite structures with Lewis acid–base matrices.
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