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Tricalcium aluminate (C 3 A) is a major phase of Portland cement clinker and some dental root filling cements. An accurate all-atom force field is introduced to examine structural, surface, and hydration properties as well as organic interfaces to overcome challenges using current laboratory instrumentation. Molecular dynamics simulation demonstrates excellent agreement of computed structural, thermal, mechanical, and surface properties with available experimental data. The parameters are integrated into multiple potential energy expressions, including the PCFF, CVFF, CHARMM, AMBER, OPLS, and INTERFACE force fields. This choice enables the simulation of a wide range of inorganic-organic interfaces at the 1 to 100 nm scale at a million times lower computational cost than DFT methods. Molecular models of dry and partially hydrated surfaces are introduced to examine cleavage, agglomeration, and the role of adsorbed organic molecules. Cleavage of crystalline tricalcium aluminate requires approximately 1300 mJ m −2 and superficial hydration introduces an amorphous calcium hydroxide surface layer that reduces the agglomeration energy from approximately 850 mJ m −2 to 500 mJ m −2 , as well as to lower values upon surface displacement. The adsorption of several alcohols and amines was examined to understand their role as grinding aids and as hydration modifiers in cement. The molecules mitigate local electric fields through complexation of calcium ions, hydrogen bonds, and introduction of hydrophobicity upon binding. Molecularly thin layers of about 0.5 nm thickness reduce agglomeration energies to between 100 and 30 mJ m −2 . Molecule-specific trends were found to be similar for tricalcium aluminate and tricalcium silicate. The models allow quantitative predictions and are a starting point to provide fundamental understanding of the role of C 3 A and organic additives in cement. Extensions to impure phases and advanced hydration stages are feasible.

Recent investigations have revealed the great potential of Raman spectroscopy for the characterization of clinker minerals and commercial Portland cements. The usefulness of this technique for the identification of anhydrous, hydrated, and carbonated phases in cement-based materials has been demonstrated. In the present work, the application of micro-Raman spectroscopy for the characterization of the main clinker phases of calcium aluminate cements and calcium sulfoaluminate cement is explored. The main stable hydrated phases as well as several important carbonated phases are investigated. Raman measurements on the following phases are reported: (i) pure, unhydrated phases: CA, C12A7, CA2, C2AS, cubic-C3A, C4AF, and C4A3inline image; (ii) hydrated phases: ettringite, monosulfoaluminate, and hydrogarnet (C3AH6); (iii) carboaluminate phases: hemicarboaluminate and monocarboaluminate. The present results, which are discussed in terms of the internal vibrational modes of the aluminate, carbonate, and sulfate molecular groups as well as stretching O–H vibrations, show the ability of Raman spectroscopy to identify the main hydrated and unhydrated phases in the aluminate and sulfoaluminate cements. The Raman spectra obtained in this work provide an extended database to the existing data published in the literature.Peer ReviewedPostprint (published version

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This experimental research analyzes the mechanical performance and durability of façade pieces based on Portland cement matrix and flax nonwovens as reinforcement. Two types of pozzolanic additions (silica fume and metakaolin) combined with nonwovens subjected to different treatments to decrease their water absorption are analyzed as potential materials for fiber-cement sheets for building envelopes with high strength and durability. For this purpose, on the one hand, the mechanical performance and chemical composition of various ternary compositions were studied. On the other hand, various treatments were performed on the nonwovens and the nonwoven-matrix adherence was also analyzed. Finally, composites were prepared from some selected treated nonwovens and matrix mixtures, and their mechanical properties and durability were evaluated under four-point bending tests after 28 days of curing in a humidity chamber and after accelerated aging. The composites developed with the treated nonwovens presented very high performance combined with enough durability to be potential candidates for the development of sustainable materials for building envelopes. Highlights-Mechanical performance and durability of OPC/flax nonwovens composites for façade pieces is explored -The effect of two pozzolanic additions combined with nonwoven treatment is evaluated -Significant improvements in the durability using treated nonwovens 3