Abstract Coupling of organic and inorganic chemistry presents a new degree of freedom in nano-engineering of thermo-mechanical properties of cement-based materials. Despite these vast technological benefits, molecular scale cross-linking of calcium-silicate-hydrate (C-S-H) gel with organic molecules still presents a significant challenge. Herein, we report experimental results on sol-gel synthesis, structure and morphology of nanocrystalline C-S-H cross-linked with dipodal organosilanes. These novel organic-inorganic gels have layered turbostratic molecular structure with similarities to C-S-H precipitating in hydrating cement paste. The organic molecules' chain length controls the interlayer spacing, which shows little to no shrinkage upon dehydration up to 105 °C. However, the structure gets distorted in the basal crystallite plane, in which dimer and trimer Si-polyhedra structures condense on a 2D hexagonal Ca-polyhedra layer. Cross-linked C-S-H gels display plate-like morphology with tendency toward stacking into agglomerates at the larger scale. If successfully realized in cement environment, e.g. high concentration seed, such novel organic-inorganic C-S-H gels could potentially provide cement-based matrices with unique properties unmatched by classical inorganic systems.

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与双足有机硅烷交联的硅酸钙水合物的结构和形态

摘要 有机和无机化学的结合为水泥基材料热机械性能的纳米工程提供了一个新的自由度。尽管有这些巨大的技术优势，水化硅酸钙 (CSH) 凝胶与有机分子的分子级交联仍然是一个重大挑战。在此，我们报告了与双足有机硅烷交联的纳米晶 CSH 的溶胶-凝胶合成、结构和形态的实验结果。这些新型有机-无机凝胶具有层状乱层分子结构，与水化水泥浆中的 CSH 沉淀相似。有机分子的链长控制着层间距，脱水至 105 °C 时几乎没有收缩。然而，结构在基础微晶平面中扭曲，其中二聚体和三聚体硅多面体结构凝聚在二维六边形钙多面体层上。交联的 CSH 凝胶显示出类似板状的形态，并有在更大范围内堆积成团块的趋势。如果在水泥环境中成功实现，例如高浓度种子，这种新型有机-无机 CSH 凝胶有可能提供具有经典无机系统无法比拟的独特性能的水泥基基质。