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1.
Proc Natl Acad Sci U S A ; 120(32): e2304318120, 2023 Aug 08.
Artigo em Inglês | MEDLINE | ID: mdl-37523534

RESUMO

The large-scale implementation of renewable energy systems necessitates the development of energy storage solutions to effectively manage imbalances between energy supply and demand. Herein, we investigate such a scalable material solution for energy storage in supercapacitors constructed from readily available material precursors that can be locally sourced from virtually anywhere on the planet, namely cement, water, and carbon black. We characterize our carbon-cement electrodes by combining correlative EDS-Raman spectroscopy with capacitance measurements derived from cyclic voltammetry and galvanostatic charge-discharge experiments using integer and fractional derivatives to correct for rate and current intensity effects. Texture analysis reveals that the hydration reactions of cement in the presence of carbon generate a fractal-like electron-conducting carbon network that permeates the load-bearing cement-based matrix. The energy storage capacity of this space-filling carbon black network of the high specific surface area accessible to charge storage is shown to be an intensive quantity, whereas the high-rate capability of the carbon-cement electrodes exhibits self-similarity due to the hydration porosity available for charge transport. This intensive and self-similar nature of energy storage and rate capability represents an opportunity for mass scaling from electrode to structural scales. The availability, versatility, and scalability of these carbon-cement supercapacitors opens a horizon for the design of multifunctional structures that leverage high energy storage capacity, high-rate charge/discharge capabilities, and structural strength for sustainable residential and industrial applications ranging from energy autarkic shelters and self-charging roads for electric vehicles, to intermittent energy storage for wind turbines and tidal power stations.

2.
PNAS Nexus ; 2(3): pgad052, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-37007709

RESUMO

Addressing the existing gap between currently available mitigation strategies for greenhouse gas emissions associated with ordinary Portland cement production and the 2050 carbon neutrality goal represents a significant challenge. In order to bridge this gap, one potential option is the direct gaseous sequestration and storage of anthropogenic CO2 in concrete through forced carbonate mineralization in both the cementing minerals and their aggregates. To better clarify the potential strategic benefits of these processes, here, we apply an integrated correlative time- and space-resolved Raman microscopy and indentation approach to investigate the underlying mechanisms and chemomechanics of cement carbonation over time scales ranging from the first few hours to several days using bicarbonate-substituted alite as a model system. In these reactions, the carbonation of transient disordered calcium hydroxide particles at the hydration site leads to the formation of a series of calcium carbonate polymorphs including disordered calcium carbonate, ikaite, vaterite, and calcite, which serve as nucleation sites for the formation of a calcium carbonate/calcium-silicate-hydrate (C-S-H) composite, and the subsequent acceleration of the curing process. The results from these studies reveal that in contrast to late-stage cement carbonation processes, these early stage (precure) out-of-equilibrium carbonation reactions do not compromise the material's structural integrity, while allowing significant quantities of CO2 (up to 15 w%) to be incorporated into the cementing matrix. The out-of-equilibrium carbonation of hydrating clinker thus provides an avenue for reducing the environmental footprint of cementitious materials via the uptake and long-term storage of anthropogenic CO2.

3.
Materials (Basel) ; 14(22)2021 Nov 18.
Artigo em Inglês | MEDLINE | ID: mdl-34832370

RESUMO

Recently, the research of innovative building materials is focused on applying supplementary materials in the form of micro- and nanopowders in cementitious composites due to the growing insistence on sustainable development. Considering above, in paper, a research on the effect of microsilica and SiO2 nanoparticles addition to cement paste, designed with Andreasen and Andersen (AA) packing density model (PDM), in terms of its physical and mechanical properties was conducted. Density, porosity, compressive strength, hardness, and modulus of indentation were investigated and compared regarding different amount of additives used in cement paste mixes. Microstructure of the obtained pastes was analyzed. The possibility of negative influence of alkali-silica reaction (ASR) on the mechanical properties of the obtained composites was analyzed. The results of the conducted investigations were discussed, and conclusions, also practical, were presented. The obtained results confirmed that the applied PDM may be an effective tool in cement paste design, when low porosity of prepared composite is required. On the other hand, the application of AA model did not bring satisfactory results of mechanical performance as expected, what was related, as shown by SEM imaging, with inhomogeneous dispersion of microsilica, and creation of agglomerates acting as reactive aggregates, what as a consequence caused ASR reaction, crack occurrence and lowered mechanical properties. Finally, the study found that the use of about 7.5% wt. of microsilica is the optimum in regards to obtain low porosity, while, to achieve improved mechanical properties, the use of 4 wt. % of microsilica seems to be optimal, in the case of tested cement pastes.

4.
Materials (Basel) ; 11(8)2018 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-30087261

RESUMO

When understanding the effect of the morphology of coarse aggregate on the properties of a fresh concrete mixture, the strength and deformability of self-compacting high-performance fibre-reinforced concrete (SCHPFRC) can be seen to be critical for its performance. In this research, regular and irregular grains were separated from granite coarse aggregate. The morphology of these grains was described while using digital image analysis. As a result, the aspect ratio, roundness and area ratio were determined in order to better understand this phenomenon. Then, the principal rheological, physical, and mechanical properties of SCHPFRC were determined. The obtained results indicated that the morphology of the grains of coarse aggregate has an impact on the strength and stiffness properties of SCHPFRC. Moreover, significant differences in the transverse strain of concretes were observed. The morphology of the coarse aggregate also has an impact on the rheological parameters of a fresh concrete mixture. To better understand this phenomenon, the hypothesized mechanism of the formation of SCHPFRC caused by different morphology of coarse aggregate was proposed at the end of the article.

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