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Nanotechnology enables the design of materials with outstanding performance. A key element of nanotechnology is the ability to manipulate and control matter on the nanoscale to achieve a certain desired set of specific properties. Here, we discuss recent insight into the formation mechanisms of inorganic nanoparticles during precipitation reactions. We focus on calcium carbonate, and describe the various transient stages potentially occurring on the way from the dissolved constituent ions to finally stable macrocrystals-including solute ion clusters, dense liquid phases, amorphous intermediates, and nanoparticles. The role of polymers in nucleating, templating, stabilizing, and/or preventing these structures is outlined. As a specific example for applied nanotechnology, the properties of cement are shown to be determined by the formation and interlocking of calcium-silicate-hydrate nanoplatelets. The aggregation of these platelets into mesoscale architectures can be controlled with polymers.

In a book published in 1906, Richard Meade outlined the history of portland cement up to that point1. Since then there has been great progress in portland cement-based construction materials technologies brought about by advances in the materials science of composites and the development of chemical additives (admixtures) for applications. The resulting functionalities, together with its economy and the sheer abundance of its raw materials, have elevated ordinary portland cement (OPC) concrete to the status of most used synthetic material on Earth. While the 20th century was characterized by the emergence of computer technology, computational science and engineering, and instrumental analysis, the fundamental composition of portland cement has remained surprisingly constant. And, although our understanding of ordinary portland cement (OPC) chemistry has grown tremendously, the intermediate steps in hydration and the nature of calcium silicate hydrate (C-S-H)*, the major product of OPC hydration, remain clouded in uncertainty. Nonetheless, the century also witnessed great advances in the materials technology of cement despite the uncertain understanding of its most fundamental components. Unfortunately, OPC also has a tremendous consumption-based environmental impact, and concrete made from OPC has a poor strength-to-weight ratio. If these challenges are not addressed, the dominance of OPC could wane over the next 100 years. With this in mind, this paper envisions what the 21st century holds in store for OPC in terms of the driving forces that will shape our continued use of this material. Will a new material replace OPC, and concrete as we know it today, as the preeminent infrastructure construction material?

Despite a millennial history and the ubiquitous presence of cement in everyday life, the molecular processes underlying its hydration behavior, like the formation of calcium–silicate–hydrate (C–S–H), the binding phase of concrete, are mostly unexplored. Using time-resolved potentiometry and turbidimetry combined with dynamic light scattering, small-angle X-ray scattering, and cryo-TEM, we demonstrate C–S–H formation to proceed via a complex two-step pathway. In the first step, amorphous and dispersed spheroids are formed, whose composition is depleted in calcium compared to C–S–H and charge compensated with sodium. In the second step, these amorphous spheroids crystallize to tobermorite-type C–S–H. The crystallization is accompanied by a sodium/calcium cation exchange and aggregation. Understanding the formation of C–S–H via amorphous liquid precursors may allow for a better understanding of the topography of the nucleation in cement paste and thus the percolation of hydration products leading to the mechanical setting as well as the retarding effect of known chemical species like aluminum ions and polycarboxylate ethers.

Controlled aggregation of polymer-stabilized calcium silicate hydrate nanoparticles leads to elastic cementitious materials.

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15The atomic structure of calcium-silicate-hydrate (C1,67-S-Hx) has been investigated by 16 theoretical methods in order to establish a better insight into its structure. Three models for C-17 S-H all derived from tobermorite are proposed and a large number of structures were created 18 within each model by making a random distribution of silica oligomers of different size 19 within each structure. These structures were subjected to structural relaxation by geometry 20 optimization and molecular dynamics steps. That resulted in a set of energies within each 21 model. Despite an energy distribution between individual structures within each model, 22 significant energy differences are observed between the three models. The C-S-H model 1 related to the lowest energy is considered as the most probable. It turns out to be characterized 2 by the distribution of dimeric and pentameric silicate and the absence of monomers. This 3 model has mass density which is the closest to the experimental one. 4 5