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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Use of Lignin-Based Admixture as Water Reducer (WRA) for Tailoring the Rheological Properties of Mortars for 3D-Printing

Efforts towards decarbonizing construction materials and industrial processes related to cement and concrete can be aided via multifaceted approaches that target alternative admixtures as well as precision control of fabrication. Chemical admixtures for water reduction have played a crucial role in the development of advanced mortar and concrete mixtures. Newer biomass processing techniques developed for aviation fuel production from corn stover biomass produce a highly reactive lignin byproduct that is suitable for chemical modifications to mimic the properties of commonly used polycarboxylate ethers (PCEs) with a smaller carbon footprint. These lignin-based plasticizers developed at NREL can be used in place of petrochemical-derived superplasticizers to tailor the rheological properties of cement-based systems for applications such as additive manufacturing while reducing the carbon intensity of the concrete mix. Lignosulfonates derived from paper pulping were historically used as water reducers only to be displaced with the rise of PCEs. The present study examines the use of a NREL produced lignin-based water reducing admixture (WRA), in cement pastes and mortar mixtures for 3D-printing at small- (mm) scale. The experimental program consisted of different formulations of oxidized lignin-based WRAs added in variable dosages to cement pastes with a fixed water-to-cement ratio. The objective is to achieve an appropriate workability, extrudability and buildability of mortar mixtures to produce 3D-printed specimens. The rheological characterization was performed to compare the initial yield stress and viscosity of the different mixtures with lignin-based admixture with respect to conventional PCE superplasticizers. The rheological characterization shows that the proposed material act as an effective water-reducer in cement systems, affecting the yield stress, plastic viscosity, and structuration rate of the mixtures evaluated. On the other hand, the effect on early hydration process of the cement pastes containing lignin-based admixtures is comparable to conventional superplasticizers.

3D-printing↗
DOE OSTI2026

The future of subsurface monitoring: AEC’s breakthroughs in CCS technology

Carbon capture and storage (CCS) has emerged as a key solution in the fight against climate change. However, for CCS to succeed, it is crucial to ensure that the sequestered CO2 stays safely trapped underground. The U.S. Department of Energy (DOE) has emphasized the need for advancements in subsurface monitoring, measurement, reporting, and verification. Aside from caprock integrity failure, the other primary failure points usually involve defective cement in the casing annulus of wellbores or plugged and abandoned wells. In addition, many energy producers (e.g., oil and gas, geothermal) and storage and disposal operators (e.g., H2 and water) must deal with the same issue. Poorly placed or degraded cement can create pathways for gas or fluid to escape from casing annuli and in plugged and abandoned or orphan wells, posing environmental risks. Yet, a reliable and cost-effective way to monitor cement and well integrity over multiple decades is still unavailable. Traditional geophysical methods like 4D seismic imaging and surface-based electromagnetic monitoring lack the resolution and accuracy for detecting these types of failures (Vasco et al., 2022; Fawad and Mondol, 2021). Wireline logging is expensive to run continuously and is obtrusive to the operation. While fiber optics can potentially be a solution, its bulkiness can significantly compromise the cement's integrity. To address these challenges, the Advanced Energy Consortium (AEC) at The University of Texas at Austin’s Bureau of Economic Geology (the Bureau) has been pioneering research in subsurface monitoring using its portfolio of distributed autonomous microfabricated sensors for harsh subsurface environments since 2008. A class of these microsensors [System on a Chip (SoC)] can be mixed in cement and permanently placed without compromising the cement column; the sensors would then communicate with each other or a data acquisition (DAQ) master node. Another class of the AEC microsensors can be fully autonomous, with rechargeable micro-batteries capable of exceeding 100°C, flash memory, and, currently, a pressure and temperature sensor. They are designed to circulate in mud, geothermal fluids, U-loops, or pipelines. They can log data into memory and are unobtrusive to operations. Our team has been working on a multi-year DOE-funded project (DE-FE0031856)—supported by $2.95M in federal funding and $0.75M in cost-matching from the AEC—to demonstrate SoC sensor utility for CO2 leakage monitoring in CCS applications. This multi-institutional collaboration developed a novel sensing architecture utilizing radiofrequency (RF) microsensors embedded within the cement sheath. These sensors detect CO2 migration and are interrogated via a Smart Casing Collar (SCC).

58 GEOSCIENCES↗
DOE OSTI2014

Effect of blast furnace slag on self-healing of microcracks in cementitious materials

The physico-chemical process of self-healing in blast furnace slag cement paste was investigated in this paper. With a high slag content i.e., 66% in cement paste and saturated Ca(OH)₂ solution as activator, it was found that the reaction products formed in cracks are composed of C-S-H, ettringite, hydrogarnet and OH–hydrotalcite. The fraction of C-S-H in the reaction products is much larger than the other minerals. Large amount of ettringite formed in cracks indicates the leaching of SO₄⁻² ions from the bulk paste and consequently the recrystallization. Self-healing proceeds fast within 50 h and then slows down. According to thermodynamic modeling, when the newly formed reaction products are carbonated, the filling fraction of crack increases first and then decreases. Low soluble minerals such as silica gel, gibbsite and calcite are formed. Compared to Portland cement paste, the potential of self-healing in slag cement paste is higher when the percentage of slag is high. Highlights: • Self-healing reaction products in slag cement paste were characterized. • Self-healing reaction products formed in time were quantified with image analysis. • Self-healing in slag cement paste was simulated with a reactive transport model. • Effect of carbonation on self-healing was investigated by thermodynamic modeling. • Effect of slag on self-healing was discussed based on experiments and simulation.

36 MATERIALS SCIENCE↗
DOE OSTI2014

A thermodynamic model for C-(N-)A-S-H gel: CNASH{sub s}s. Derivation and validation

The main reaction product in Ca-rich alkali-activated cements and hybrid Portland cement (PC)-based materials is a calcium (alkali) aluminosilicate hydrate (C-(N-)A-S-H) gel. Thermodynamic models without explicit definitions of structurally-incorporated Al species have been used in numerous past studies to describe this gel, but offer limited ability to simulate the chemistry of blended PC materials and alkali-activated cements. Here, a thermodynamic model for C-(N-)A-S-H gel is derived and parameterised to describe solubility data for the CaO–(Na{sub 2}O,Al{sub 2}O{sub 3})–SiO{sub 2}–H{sub 2}O systems and alkali-activated slag (AAS) cements, and chemical composition data for C-A-S-H gels. Simulated C-(N-)A-S-H gel densities and molar volumes are consistent with the corresponding values reported for AAS cements, meaning that the model can be used to describe chemical shrinkage in these materials. Therefore, this model can provide insight into the chemistry of AAS cements at advanced ages, which is important for understanding the long-term durability of these materials.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Microstructural effects in the simulation of creep of concrete

The influence of the microstructure on the visco-elastic properties of concrete is investigated using finite element simulations at the meso-scale. We first derive a constitutive law for the creep of the cement paste which accounts for both recoverable and permanent deformations, as well as the influence of temperature and internal relative humidity. The model is calibrated on a set of experiments at the cement paste scale, and then validated after upscaling to the concrete scale. The model is then applied to study the influence of the microstructure on the macroscopic creep of concrete. We show that materials with finer particles exhibit less creep, and that the anisotropy of creep can be explained with the shape and orientation of the aggregates. Furthermore, the acceleration of the stress relaxation in the presence of damage is explained by the micro-mechanical interaction between the aggregates, the cement paste, and the micro-cracks.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Plastic deformation mechanism of calcium-silicate hydrates determined by deviatoric-stress Raman spectroscopy

Highlights: • C-(A-)S-H samples under stress were characterized at the bond and grain level. • Small angle scattering showed that 720 MPa reduced grain thickness by 30%. • In-situ Raman showed that cross-linked C-A-S-H slips along its intralayer. • However, in-situ Raman showed that C-S-H slips along the interlayer. • In-situ Raman also showed a growth in CaCO{sub 3}, indicating fracture in both samples. Creep of the cement matrix affects the structural stability of concrete. In Portland cements, the creep is largely controlled by the binding phase calcium-(aluminum-)silicate-hydrate, or C-(A-)S-H. This phase has a lamellar structure and under deviatoric stress aligns its c-axis with the principal stress. However, the limiting resistance to this reorientation is unknown at the nanocrystalline level. Small-angle X-ray scattering shows that the lamellae thickness decreases under 100's MPa deviatoric stress. Deviatoric stress Raman spectroscopy shows that there are two ways that this break-up can occur. If the material's silicate chains are cross-linked, then strain in SiO bonds does not increase above certain stresses, indicating a relaxation adjacent to the SiO bond. If the chains are not cross-linked, then the silicate chains are broken up by rastering against each other, introducing defects. These results show that the plastic deformation of C-(A-)S-H is relevant for Portland cement creep.

36 MATERIALS SCIENCE↗
DOE OSTI2021

The chemical and physical origin of incineration ash reactivity in cementitious systems

Incorporating industrial byproducts and waste in concrete is the key to reducing landfill usage as well as lowering the environmental footprint of cement industry. An emerging industrial byproduct which can partly replace cement is the Municipal Solid Waste Incinerator Ash (MSWI ash: residue that is left after incineration of municipal solid waste in a Waste-to-Energy facility). These ashes are predominantly calcium-rich; however, they also contain additional elements whose speciation is not known. These elements can significantly alter the hydration characteristics of a cementitious system. Here, our results suggest these ashes can accelerate as well as retard cement hydration. Specifically, Pb, Br, S, Ca, and Cl appear to accelerate cement hydration, whereas Cu, Fe, Al, Ti, Si, K, Zn, and Sr appear to retard cement hydration. Changes in hydration characteristics can have a strong bearing on the physical characteristics of cementitious systems incorporating incineration ashes. Thus, to selectively screen ashes that synergistically enhance the physical characteristics, we introduce a novel “Incineration Ash Coefficient (IAC),” which shows a strong correlation with the compressive strength (R 2 =0.79) of cement-ash binary mixtures.

42 ENGINEERING↗
DOE OSTI2015

Planning large-scale excavation and construction activities within an aerially constrained site for construction of a repository for low and short-lived intermediate level radioactive waste at the Bulgarian national disposal facility - 15372

The Bulgarian State Enterprise for Radioactive Waste Management (SERAW) is planning the construction of a near-surface repository for low and short-lived intermediate level radioactive waste, the National Disposal Facility (NDF), at the Radiana Site adjacent to the Kozloduy Nuclear Power Plant (KNPP). The Site, a rectangular area approximately 1.2 km east-west by 0.4 north-south, is located on a slopping area between the second and sixth loess terraces above the River Danube with elevations ranging from approximately +40 m to elevation +95 m. Construction of the NDF will be divided into three phases separated by approximately 20 years each. The first phase will see the construction of the primary support facilities, referred to as the Auxiliary Buildings and including the Waste Reception and Buffer Storage (WRBS) Building, and the first set of 22 reinforced concrete disposal cells and supporting infrastructure, including a network of subsurface observation galleries, the Infiltration Network Control (ICN) Galleries. Each disposal cell will be 20.15 m long by 17.05 m wide by 9.45 m in height. The disposal cells will be arranged in two parallel rows. Disposal activities will be conducted using overhead cranes installed inside of track mounted mobile roofs. Each row of disposal cells will be serviced by one mobile roof. The mobile roofs will be supported by massive concrete foundations. Construction at the site will present several logistical challenges that will need to be overcome to fully realize the NDF. First in order to begin construction of these facilities nearly 1 million 3 of soil will require excavation and handling. Consistent with requirements to minimize potential environmental impacts identified in the site Environmental Safety Assessment (EIA) excavated soil will, to the extent possible, remain onsite. Approximately three quarters of the soil can be accommodated within the site boundaries. Another challenge results from requirements imposed by the ground conditions. The sub-grade at the site, which consists primarily of loess, will require considerable improvement. To this end a 5 m thick loess-cement cushion will be constructed across much of the site. Specifically, the cushion will be required beneath the disposal cells and the WRBS Building. Construction of the loess-cement cushion in the disposal area will require detailed planning and coordination, particularly as the cushion beneath the disposal cells also contains embedded structures, including the ICN Galleries as well as massive concrete foundation beams required for the two mobile roofs. Construction of these structures will require planned interruptions in the construction of the loess-cement cushion. Specific cement types and strict quality requirements will be required for completion of the loess-cement cushion as well as for completion of the ICN Galleries. The construction planning will need to account for the large volumes of soil to be excavated as well as ensuring sufficient material supplies in terms of both quality as well as quantity. Large quantities of materials including both dry cement for mixing with the loess, and wet concrete for pouring of the mobile roof foundations are accounted for by the plan. However, even after completion of these activities additional challenges are addressed by the plan related to the contemporaneous construction management of the auxiliary buildings and the disposal cells. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Modeling the Long-Term Behavior of Cementitious Barriers - 18188

Cementitious materials are commonly included as backfill/barrier materials in geological repositories for radioactive waste. An understanding of the long-term behavior of cement-based barriers is therefore required to provide confidence in their safety functions within an environmental safety case. Geochemical modelling has been undertaken on several different radioactive waste repository concepts (and their natural/industrial analogues), to explore the nature of cement degradation over timescales relevant to postclosure safety (many tens of thousands of years to c. 1 Ma). In radionuclide transport calculations undertaken as part of performance assessments, it is typically considered that the properties of cementitious engineered barrier materials change as they degrade, potentially resulting in an increase in porosity hydraulic conductivity, and effective diffusion coefficients. However, reactive transport modelling (supported by some analogue data) suggests that, in some repository systems, a degree of clogging of the cement pore space could occur and that some advective flow paths (cracks in the barriers, fractures in the host rock) could become (to some extent) infilled by cement and rock alteration products. This could result in a reduction in water flow and contaminant transport in the vicinity of the cement-rock interface, but some uncertainties remain (especially process couplings and the nature of water flow in complex fracture networks that are becoming clogged). In addition, the armoring of fracture surfaces could result in decreased potential for diffusion of solutes into the rock matrix. It is envisaged that ongoing work will continue to improve reactive-transport model capabilities, such that the implications cement degradation has for contaminant transport can be predicted with greater confidence. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2019

Rare earth elements and radiogenic strontium isotopes in carbonate minerals reveal diagenetic influence in shales and limestones in the Appalachian Basin

Rare earth element (REE) signatures are often applied to interpret paleoenvironmental conditions in sedimentary basins, however the complicated diagenetic histories in dynamic depositional environments can affect interpretation of measured REE signatures. Prior studies on REE content in shales and limestones indicated that REE in specific mineral phases may provide unique information concerning diagenetic reactions occurring in sedimentary rocks during burial and compaction. Application of sequential extraction techniques to target REE signatures in specific mineral fractions may provide greater insight into the complex processes that occurred during diagenesis and catagenesis. Thus, using this technique, this study provides a detailed account for REE, 87 Sr/ 86 Sr, and δ 13 C in the carbonate fraction of the Marcellus Shale and adjacent formations in the Appalachian Basin. A suite of 49 rock samples collected from two cores recovered from Monongalia County, West Virginia, USA was analyzed. The results showed that the carbonate concretions in calcareous shales and carbonate cements in black shales were very distinct. The REE plus yttrium (REY) were more concentrated in the carbonate concretions than in the carbonate cements. The carbonate concretions displayed REY patterns that are closely similar to modern seawater, while MREE-enrichment was observed in the carbonate cements. Likewise, the 87 Sr/ 86 Sr values in the carbonate concretions were similar to those measured for unaltered Middle Devonian carbonates, while the 87 Sr/ 86 Sr in the carbonate cements were much more radiogenic. This observation indicates that the carbonate cement could have been inherited radiogenic 87 Sr expulsed from clays during illite-smectite transition. Overall, this study demonstrated two distinct processes involved with controlling the carbonate geochemistry within Appalachian Basin shales and limestones: one fraction displaying minimal diagenetic alteration relative to depositional conditions (carbonate concretions in calcareous shales and limestone carbonate in limestones), and another fraction displaying the evidence for extensive chemical alteration during illite-smectite transition and catagenesis (carbonate cements in black shales). Here, in addition, highly variable and significant enrichments of U and Mo demonstrate that the Union Spring member and the Lower Oatka Creek member of the Marcellus Shale in the southwestern Appalachian Basin (MSEEL site) were deposited under mainly anoxic environment whereas intermitted episodes of dysoxic to perhaps oxic conditions occurred during the deposition of the Upper Oatka Creek member.

58 GEOSCIENCES↗
DOE OSTI2020

Characterization of paste microstructure for durability properties of concrete

In this study, paste samples from different cementitious systems were characterized by using X-Ray Micro Computed Tomography (µ-CT) and Fluorescence Microscopy techniques. Quantitative and qualitative aspects of defects from paste samples were investigated to develop indicators of durability related properties of corresponding concrete samples. In the first phase of this study, hour glass shaped 3D printed molds were used to investigate five cementitious combinations consisting of three cement types (Coarse Ground portland cement, Type IL Portland Limestone Cement and Type I/II ordinary portland cement) and fly ash as a supplementary cementitious material. In the second phase, metal molds were used to compare the results of Coarse Ground portland cement with Type I ordinary portland cement, 5% of which was replaced with colloidal nanosilica. Potential correlations between paste and concrete have been presented. This work was supported by US Department of Energy and North Dakota Department of Commerce.

36 MATERIALS SCIENCE↗
DOE OSTI2019

The Role of Chemistry in Fracture Pattern Development and Opportunities to Advance Interpretations of Geological Materials

Abstract Fracture pattern development has been a challenging area of research in the Earth sciences for more than 100 years. Much has been learned about the spatial and temporal complexity inherent to these systems, but severe challenges remain. Future advances will require new approaches. Chemical processes play a larger role in opening‐mode fracture pattern development than has hitherto been appreciated. This review examines relationships between mechanical and geochemical processes that influence the fracture patterns recorded in natural settings. For fractures formed in diagenetic settings (~50 to 200 °C), we review evidence of chemical reactions in fractures and show how a chemical perspective helps solve problems in fracture analysis. We also outline impediments to subsurface pattern measurement and interpretation, assess implications of discoveries in fracture history reconstruction for process‐based models, review models of fracture cementation and chemically assisted fracture growth, and discuss promising paths for future work. To accurately predict the mechanical and fluid flow properties of fracture systems, a processes‐based approach is needed. Progress is possible using observational, experimental, and modeling approaches that view fracture patterns and properties as the result of coupled mechanical and chemical processes. A critical area is reconstructing patterns through time. Such data sets are essential for developing and testing predictive models. Other topics that need work include models of crystal growth and dissolution rates under geological conditions, cement mechanical effects, and subcritical crack propagation. Advances in machine learning and 3‐D imaging present opportunities for a mechanistic understanding of fracture formation and development, enabling prediction of spatial and temporal complexity over geologic timescales. Geophysical research with a chemical perspective is needed to correctly identify and interpret fractures from geophysical measurements during site characterization and monitoring of subsurface engineering activities.

58 GEOSCIENCES↗
DOE OSTI2015

Measurement of tritium penetration through concrete material covered by various paints coating

The present study aims at obtaining fundamental data on tritium migration in porous materials, which include soaking effect, interaction between tritium and cement paste coated with paints and transient tritium sorption in porous cement. The amounts of tritium penetrated into or released from cement paste with epoxy and urethane paint coatings were measured. The tritium penetration amounts were increased with the HTO (tritiated water) exposure time. Time to achieve a saturated value of tritium sorption was more than 60 days for cement paste coated with epoxy paint and with urethane paint, while that for cement paste without any paint coating took 2 days to achieve it. The effect of tritium permeation reduction by the epoxy paint was higher than that of the urethane. Although their paint coatings were effective for reduction of tritium penetration through the cement paste which was exposed to HTO for a short period, it was found that the amount of tritium trapped in the paints became large for a long period. Tritium penetration rates were estimated by an analysis of one-dimensional diffusion in the axial direction of a thickness of a sample. Obtained data were helpful for evaluation of tritium contamination and decontamination. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Integrated Multiphysics Modeling of Environmentally Assisted Brittle Fracture

Brittle materials, such as cement, compose major portions of built infrastructure and are vulnerable to degradation and fracture from chemo-mechanical effects. Currently, methods of modeling infrastructure do not account for the presence of a reactive environment, such as water, on the acceleration of failure. Here, we have developed methodologies and models of concrete and cement fracture that account for varying material properties, such as strength, shrinkage, and fracture toughness due to degradation or hydration. The models have been incorporated into peridynamics, non-local continuum mechanics methodology, that can model intersecting and branching brittle fracture that occurs in multicomponent brittle materials, such as concrete. Through development of new peridynamic capabilities, decalcification of cement and differential shrinkage in clay-cement composites have been evaluated, along with exemplar problems in nuclear waste cannisters and wellbores. We have developed methods to simulate multiphase phenomena in cement and cement-composite materials for energy and infrastructure applications.

36 MATERIALS SCIENCE↗
NASA NTRS2001

A Model for Formation of Dust, Soil and Rock Coatings on Mars: Physical and Chemical Processes on the Martian Surface

This model is one of many possible scenarios to explain the generation of the current surface material on Mars using chemical, magnetic and spectroscopic data From Mars and geologic analogs from terrestrial sites. One basic premise of this model is that the dust/soil units are not derived exclusively from local rocks, but are rather a product of global, and possibly remote, weathering processes. Another assumption in this model is that there are physical and chemical interactions of the atmospheric dust particles and that these two processes create distinctly different results on the surface. Physical processes distribute dust particles on rocks and drift units, forming physically-aggregated layers; these are reversible processes. Chemical reactions of the dust/soil particles create alteration rinds on rock surfaces and cohesive, crusted surface units between rocks, both of which are relatively permanent materials. According to this model the dominant components of the dust/soil particles are derived from alteration of volcanic ash and tephra, and contain primarily nanophase and poorly crystalline ferric oxides/oxyhydroxide phases as well as silicates. These phases are the alteration products that formed in a low moisture environment. These dust/soil particles also contain a smaller amount of material that was exposed to more water and contains crystalline ferric oxides/oxyhydroxides, sulfates and clay silicates. These components could have formed through hydrothermal alteration at steam vents or fumeroles, thermal fluids, or through evaporite deposits. Wet/dry cycling experiments are presented here on mixtures containing poorly crystalline and crystalline ferric oxides/oxyhydroxides, sulfates and silicates that range in size from nanophase to 1-2 pm diameter particles. Cemented products of these soil mixtures are formed in these experiments and variation in the surface texture was observed for samples containing smectites, non-hydrated silicates or sulfates. Reflectance spectra were measured of the initial particulate mixtures, the cemented products and ground versions of the cemented material. The spectral contrast in the visible/near-infrared and mid-infrared regions is significantly reduced for the cemented material compared to the initial soil, and somewhat reduced for the ground, cemented soil compared to the initial soil. The results of this study suggest that diurnal and seasonal cycling on Mars will have a profound effect on the texture and spectral properties of the dust/soil particles on the surface. The model developed in this study provides an explanation for the generation of cemented or crusted soil units and rock coatings on Mars and may explain albedo variations on the surface observed near large rocks or crater rims.

Bishop, Janice↗
DOE OSTI2015

Preparation and characterization of a hybrid alkaline binder based on a fly ash with no commercial value

Alkali-activated Portland fly ash cement (FA/OPC) and alkali activated blast furnace slag-fly ash cement (FA/GBFS) were prepared using 70% of a low quality fly ash (FA). The low quality is associated with a high content of unburned material (loss of ignition of 14.6%). The hybrid cements were activated by the alkaline solution in order to obtain an overall SiO 2 /Al 2 O 3 molar ratio of 5.0 and 6.0 and unique overall Na 2 O/SiO 2 molar ratio of 0.21. The microstructural characterization of the blended pastes generated in the systems showed the coexistence of amorphous gels C-A-S-H and N-A-S-H gels in the hybrid systems. The addition of OPC or GBFS increases the compressive strength (at 28 days of curing) up to 127% compared with the geopolymer systems based only on FA used in this study. The content of silicates soluble also plays an important role in the reaction products and higher SiO 2 /Al 2 O 3 lead to obtain higher mechanical performance and denser structure. The results obtained show that these hybrid cements are an effective way for valorization the waste used in this study for the production of high strength and low-carbon footprint cement-type material.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Carbonation and CO{sub 2} uptake of concrete

This study developed a reliable procedure to assess the carbon dioxide (CO{sub 2}) uptake of concrete by carbonation during the service life of a structure and by the recycling of concrete after demolition. To generalize the amount of absorbable CO{sub 2} per unit volume of concrete, the molar concentration of carbonatable constituents in hardened cement paste was simplified as a function of the unit content of cement, and the degree of hydration of the cement paste was formulated as a function of the water-to-cement ratio. The contribution of the relative humidity, type of finishing material for the concrete surface, and the substitution level of supplementary cementitious materials to the CO{sub 2} diffusion coefficient in concrete was reflected using various correction factors. The following parameters varying with the recycling scenario were also considered: the carbonatable surface area of concrete crusher-runs and underground phenomena of the decreased CO{sub 2} diffusion coefficient and increased CO{sub 2} concentration. Based on the developed procedure, a case study was conducted for an apartment building with a principal wall system and an office building with a Rahmen system, with the aim of examining the CO{sub 2} uptake of each structural element under different exposure environments during the service life and recycling of the building. As input data necessary for the case study, data collected from actual surveys conducted in 2012 in South Korea were used, which included data on the surrounding environments, lifecycle inventory database, life expectancy of structures, and recycling activity scenario. Ultimately, the CO{sub 2} uptake of concrete during a 100-year lifecycle (life expectancy of 40 years and recycling span of 60 years) was estimated to be 15.5%–17% of the CO{sub 2} emissions from concrete production, which roughly corresponds to 18%–21% of the CO{sub 2} emissions from the production of ordinary Portland cement. - Highlights: • CO{sub 2} uptake assessment approach owing to the concrete carbonation is developed. • An equation to directly determine the absorbable CO{sub 2} amount in concrete is proposed. • The carbonatable surface area of concrete crusher-runs for CO{sub 2} uptake is ascertained. • This study provides typical data for uptake and emission of CO{sub 2} in concrete building.

54 ENVIRONMENTAL SCIENCES↗