Carbonaceous (e.g., limestone) and aluminosilicate (e.g., calcined clay) mineral additives are routinely used to partially replace ordinary portland cement in concrete to alleviate its energy impact and carbon footprint. These mineral additives—depending on their physicochemical characteristics—alter the hydration behavior of cement; which, in turn, affects the evolution of microstructure of concrete, as well as the development of its properties (e.g., compressive strength). Numerical, reaction-kinetics models—e.g., phase boundary nucleation-and-growth models; which are based partly on theoretically-derived kinetic mechanisms, and partly on assumptions—are unable to produce a priori prediction of hydration kinetics of cement; especially in multicomponent systems, wherein chemical interactions among cement, water, and mineral additives occur concurrently. This paper introduces a machine learning-based methodology to enable prompt and high-fidelity prediction of time-dependent hydration kinetics of cement, both in plain and multicomponent (e.g., binary; and ternary) systems, using the system’s physicochemical characteristics as inputs. Based on a database comprising hydration kinetics profiles of 235 unique systems—encompassing 7 synthetic cements and three mineral additives with disparate physicochemical attributes—a random forests (RF) model was rigorously trained to establish the underlying composition-reactivity correlations. This training was subsequently leveraged by the RF model: to predict time-dependent hydration kinetics of cement in new, multicomponent systems; more »
- Publication Date:
- NSF-PAR ID:
- Journal Name:
- Scientific Reports
- Nature Publishing Group
- Sponsoring Org:
- National Science Foundation
More Like this
The dissolution kinetics of Portland cement is a critical factor in controlling the hydration reaction and improving the performance of concrete. Tricalcium silicate (C3S), the primary phase in Portland cement, is known to have complex dissolution mechanisms that involve multiple reactions and changes to particle surfaces. As a result, current analytical models are unable to accurately predict the dissolution kinetics of C3S in various solvents when it is undersaturated with respect to the solvent. This paper employs the deep forest (DF) model to predict the dissolution rate of C3S in the undersaturated solvent. The DF model takes into account several variables, including the measurement method (i.e., reactor connected to inductive coupled plasma spectrometer and flow chamber with vertical scanning interferometry), temperature, and physicochemical properties of solvents. Next, the DF model evaluates the influence of each variable on the dissolution rate of C3S, and this information is used to develop a closed-form analytical model that can predict the dissolution rate of C3S. The coefficients and constant of the analytical model are optimized in two scenarios: generic and alkaline solvents. The results show that both the DF and analytical models are able to produce reliable predictions of the dissolution rate of C3Smore »
A three-dimensional transient model for evaluating the performance of the cement-based thermoelectric modules.The thermoelectric module (TEM) is a device that integrates multiple thermoelectric (TE) elements to realize the mutual conversion of heat and power. Due to the advantages of no moving parts and flexible expansion, the application of conventional Bi2Te3-based TEM in buildings has attracted the attention of researchers. On the other hand, the TE behavior of hardened cement composites was found by combining conductive additives with cement. Therefore, a new study on cement-based TEM for building energy harvesting and emperature control is proposed. To simulate the performance of cement-based TEM, a three-dimensional heat transfer model considering temperature-dependent TEM characteristics was established. The validity of the model is verified by comparing the results with commercial simulation software and experiments. Different from the existing analytical models and commercial software, the customized model has greater scalability, optimization, and control flexibility. Through parametric studies, the model can guide the design of TEM and the development of TE cement.
Portland cement emits bright near-infrared photoluminescence that can be excited by light wavelengths ranging from at least 500–1000 nm. The emission has a peak wavelength near 1140 nm and a width of approximately 30 nm. Its source is suggested to be small particles of silicon associated with calcium silicate phases. The luminescence peak wavelength appears independent of the cement hydration state, aggregates, and mechanical strain but increases weakly with increasing temperature. It varies slightly with the type of cement, suggesting a new non-contact method for identifying cement formulations. After a thin opaque coating is applied to a cement or concrete surface, subsequent formation of microcracks exposes the substrate’s near-infrared emission, revealing the fracture locations, pattern, and progression. This damage would escape detection in normal imaging inspections. Near-infrared luminescence imaging may therefore provide a new tool for non-destructive testing of cement-based structures.
A role for terpenoid cyclization in the atom economical polymerization of terpenoids with sulfur to yield durable compositesRenewably-sourced, recyclable materials that can replace or extend the service life of existing technologies are essential to accomplish humanity's quest for sustainable living. In this contribution, remeltable composites were prepared in a highly atom-economical reaction between plant-derived terpenoid alcohols (10 wt% citronellol, geraniol, or farnesol) and elemental sulfur (90 wt%). Investigation into the microstructures led to elucidation of a mechanism for terpenoid polyene cyclization initiated by sulfur-centered radicals. The formation of these cyclic structures contributes significantly to understanding the mechanical properties of the materials and the extent to which linear versus crosslinked network materials are formed. The terpenoid–sulfur composites can be thermally processed at low temperatures of 120 °C without loss of mechanical properties, and the farnesol–sulfur composite so processed exhibits compressive strength 70% higher than required of concrete for residential building. The terpenoid–sulfur composites also resist degradation by oxidizing acid under conditions that disintegrate many commercial composites and cements. In addition to being stronger and more chemically resistant than some commercial products, the terpenoid–sulfur composites can be used to improve the acid resistance of mineral-based Portland cement as well. These terpenoid–sulfur composites thus hold promise as elements of sustainable construction on their own or as additives to extend themore »
Alkali-activated materials: the role of molecular-scale research and lessons from the energy transition to combat climate changeAlternative (i.e., non-Portland) cements, such as alkali-activated materials, have gained significant interest from the scientific community due to their proven CO2 savings compared with Portland cement together with known short-term performance properties. However, the concrete industry remains dominated by Portland cement-based concrete. This Letter explores the technical and non-technical hurdles preventing implementation of an alternative cement, such as alkali-activated materials, in the concrete industry and discusses how these hurdles can be overcome. Specifically, it is shown that certain technical hurdles, such as a lack of understanding how certain additives affect setting of alkali-activated materials (and Portland cement) and the absence of long-term in-field performance data of these sustainable cements, can be mitigated via the use of key molecular- and nano-scale experimental techniques to elucidate dominant material characteristics, including those that control long-term performance. In the second part of this Letter the concrete industry is compared and contrasted with the electricity generation industry, and specifically the transition from one dominant technology (i.e., coal) to a diverse array of energy sources including renewables. It is concluded that financial incentives and public advocacy (akin to advocacy for renewables in the energy sector) would significantly enhance uptake of alternative cements in the concrete industry.