Research ArticleMATERIALS SCIENCE

Mesocrystalline calcium silicate hydrate: A bioinspired route toward elastic concrete materials

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Science Advances  29 Nov 2017:
Vol. 3, no. 11, e1701216
DOI: 10.1126/sciadv.1701216
  • Fig. 1 TEM analysis of C-S-H.

    (A) Cryo-TEM of colloidally stabilized C-S-H crystallites at pH 12 and (B) TEM analysis of aggregated C-S-H crystallites in the absence of stabilizing agents. The approximate literature known size of 60 × 30 × 5 nm3 (36) can be assumed in both micrographs.

  • Fig. 2 Polarized optical and scanning electron micrographs of C-S-H mesocrystals.

    (A) to (C) were obtained from approach A, and (D) to (F) from approach B. For (A), (D), and (E), same colors indicate same orientations. The POM analysis suggests a long-range order of the agglomerated C-S-H crystallites over several hundreds of micrometers. (B) reveals a secondary structuring of the C-S-H superstructures, whereas (C) and (F) show the alignment of the single C-S-H crystallites into layers, and no microporosity can be detected.

  • Fig. 3 TEM analysis of the mesocrystals obtained from approach A.

    (A) reveals single crystalline scattering behavior indicating a perfect mutual alignment of the C-S-H nanoparticles in three-dimension (3D). (B) shows the existence of single-isolated C-S-H crystallites at the edge. Because the building blocks are not fused together whereas they scatter like single crystals, the obtained agglomerates are mesocrystals.

  • Fig. 4 Visualization of the pronounced flexibility and elasticity of a C-S-H mesocrystal lever prepared by FIB (focused ion beam).

    (A) to (F) Picture series of the bending video (available as movie S1) under the scanning electron microscope. The elasticity is revealed because the C-S-H mesocrystal cantilever fully relaxes after the application of a mechanical stress by a micromanipulator (upper left corner). The dashed line in (F) indicates the position of the C-S-H mesocrystal cantilever before bending. Scale bars, 10 μm.

Supplementary Materials

  • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/3/11/e1701216/DC1

    table S1. Mechanical properties of nacre and typical nacre-like layered nanocomposites.

    table S2. Colloidal stability of C-S-H in the presence of different copolymers at various conditions.

    fig. S1. Chemical structures of C-S-H stabilizing polymers.

    fig. S2. AUC measurements of PVP-co-PAA–stabilized C-S-H nanoplates.

    fig. S3. Strategy for the formation of nanostructured hybrid C-S-H.

    fig. S4. Dynamic light scattering of growing C-S-H mesocrystals.

    fig. S5. Evaluation of the mesocrystalline domain sizes of self-assembled C-S-H crystals (approach A).

    fig. S6. Wide-angle x-ray pattern of filtered polymer-stabilized C-S-H nanoplates (red curve) and obtained mesocrystals from pH increase (approach A, black curve) compared to C-S-H from pozzolanic reaction with CaO and SiO2 (Ca/Si = 1) (green curve).

    fig. S7. Thermogravimetric analysis of C-S-H mesocrystals.

    fig. S8. Schematical illustration of the two differently performed nanoindentation experiments on C-S-H mesocrystals from approach A.

    fig. S9. Ashby plot comparing the mechanical properties of the C-S-H mesocrystals (approach A) with various materials.

    fig. S10. SEM images of a cantilever beam used in the bending tests with the applied load perpendicular to the crystal layer planes.

    fig. S11. Schematic illustration of in-situ bending experiments.

    fig. S12. Dimensions of a cantilever beam used in the bending tests with the load applied perpendicular to the crystal layers.

    fig. S13. SEM images of a cantilever beam used in the bending tests with the load applied parallel to the crystal layers.

    movie S1. Bending test of mesocrystals obtained from pH increase to pH 12.8 under the scanning electron microscope.

    movie S2. Bending test of the same mesocrystals such as in movie S1 except that the applied stress is parallel to the crystal layer planes.

    References (3749)

  • Supplementary Materials

    This PDF file includes:

    • table S1. Mechanical properties of nacre and typical nacre-like layered nanocomposites.
    • table S2. Colloidal stability of C-S-H in the presence of different copolymers at various conditions.
    • fig. S1. Chemical structures of C-S-H stabilizing polymers.
    • fig. S2. AUC measurements of PVP-co-PAA–stabilized C-S-H nanoplates.
    • fig. S3. Strategy for the formation of nanostructured hybrid C-S-H.
    • fig. S4. Dynamic light scattering of growing C-S-H mesocrystals.
    • fig. S5. Evaluation of the mesocrystalline domain sizes of self-assembled C-S-H crystals (approach A).
    • fig. S6. Wide-angle x-ray pattern of filtered polymer-stabilized C-S-H nanoplates (red curve) and obtained mesocrystals from pH increase (approach A, black curve) compared to C-S-H from pozzolanic reaction with CaO and SiO2
      (Ca/Si = 1) (green curve).
    • fig. S7. Thermogravimetric analysis of C-S-H mesocrystals.
    • fig. S8. Schematical illustration of the two differently performed nanoindentation experiments on C-S-H mesocrystals from approach A.
    • fig. S9. Ashby plot comparing the mechanical properties of the C-S-H mesocrystals (approach A) with various materials.
    • fig. S10. SEM images of a cantilever beam used in the bending tests with the applied load perpendicular to the crystal layer planes.
    • fig. S11. Schematic illustration of in-situ bending experiments.
    • fig. S12. Dimensions of a cantilever beam used in the bending tests with the load applied perpendicular to the crystal layers.
    • fig. S13. SEM images of a cantilever beam used in the bending tests with the load applied parallel to the crystal layers.
    • Legends for movies S1 and S2
    • References (37–49)

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    Other Supplementary Material for this manuscript includes the following:S

    • movie S1 (.mp4 format). Bending test of mesocrystals obtained from pH increase to pH 12.8 under the scanning electron microscope.
    • movie S2 (.mp4 format). Bending test of the same mesocrystals such as in movie S1 except that the applied stress is parallel to the crystal layer planes.

    Files in this Data Supplement: