“Cement is the most-used material on the planet,” Pellenq says, noting that its present usage is estimated to be three times that of steel. “There’s no other solution to sheltering mankind in a durable way — turning liquid into stone in 10 hours, easily, at room temperature. That’s the magic of cement.”
In conventional cements, Pellenq explains, the calcium-to-silica ratio ranges anywhere from about 1.2 to 2.2, with 1.7 accepted as the standard. But the resulting molecular structures have never been compared in detail. Pellenq and his colleagues built a database of all these chemical formulations, finding that the optimum mixture was not the one typically used today, but rather a ratio of about 1.5.
As the ratio varies, he says, the molecular structure of the hardened material progresses from a tightly ordered crystalline structure to a disordered glassy structure. They found the ratio of 1.5 parts calcium for every one part silica to be “a magical ratio,” Pellenq says, because at that point the material can achieve “two times the resistance of normal cement, in mechanical resistance to fracture, with some molecular-scale design.”
Effect of C/S ratio on the molecular structure of C-S-H at the nanoscale.
The findings, Pellenq adds, were “validated against a large body of experimental data.” Since emissions related to concrete production are estimated to represent 5 to 10 percent of industrial greenhouse-gas emissions, he says, “any reduction in calcium content in the cement mix will have an impact on the CO2.” In fact, he says, the reduction in carbon emissions could be as much as 60 percent.
In addition to the overall improvement in mechanical strength, Pellenq says, because the material would be more glassy and less crystalline, there would be “no residual stresses in the material, so it would be more fracture-resistant.”
Global cement production is 4 billion tons per year and has doubled in the last ten years. General purpose concrete is created using a 1:2:3 ratio of cement to sand to gravel by volume. So there is 6 times more concrete versus cement.
Despite its ubiquitous presence in the built environment, concrete’s molecular-level properties are only recently being explored using experimental and simulation studies. Increasing societal concerns about concrete’s environmental footprint have provided strong motivation to develop new concrete with greater specific stiffness or strength (for structures with less material). Herein, a combinatorial approach is described to optimize properties of cement hydrates. The method entails screening a computationally generated database of atomic structures of calcium-silicate-hydrate, the binding phase of concrete, against a set of three defect attributes: calcium-to-silicon ratio as compositional index and two correlation distances describing medium-range silicon-oxygen and calcium-oxygen environments. Although structural and mechanical properties correlate well with calcium-to-silicon ratio, the cross-correlation between all three defect attributes reveals an indentation modulus-to-hardness ratio extremum, analogous to identifying optimum network connectivity in glass rheology. We also comment on implications of the present findings for a novel route to optimize the nanoscale mechanical properties of cement hydrate.
SOURCE- MIT.edu, Nature Communications
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