Semi-dry natural carbonation at different relative humidities: Degree of carbonation and reaction kinetics of calcium hydrates in cement paste
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Ground hydrated cement pastes were carbonated at different relative humidities (RH) under atmospheric CO2 concentrations to determine the effect of RH on the degree of carbonation (DoC) and reaction rates. The carbonation kinetics of each calcium-containing hydrate exhibited an initial rapid chemical-reaction-limited stage, followed by a significantly slower phase. DoC values plateaued after 200 days of carbonation, reaching 78% at 95% RH and 34% at 33% RH, aligning with EN 16757 values for sheltered outdoor and indoor environments, respectively. When the samples reached a stable DoC at a given RH, further carbonation occurred upon exposure to higher RH, implying that the DoC was governed by the highest RH to which the samples had been exposed. The phase assemblage was also affected, approaching thermodynamic equilibrium at higher RH but deviating at lower RH due to the formation of local equilibria and the presence of meta-stable phases.
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This migration behavior of calcium has been previously observed by Saeki et al. via analysis of elemental maps obtained using energy dispersive X-ray spectroscopy for OPC carbonated at 95% relative humidity and natural CO2 levels (~450-470 ppm) for 60 days.
“This migration behavior of calcium has been previously observed by Saeki et al. via analysis of elemental maps obtained using energy dispersive X-ray spectroscopy for OPC carbonated at 95% relative humidity and natural CO2 levels (~450–470 ppm) for 60 days73.”
From Spatially resolved nanostructural analysis of disordered phases in carbonated alkali-activated slag (2025) · cites this paper as [73]
Calcium migration is thought to be enhanced in wet conditions (i.e., saturated pores) and at ambient CO2 levels, where CO2 diffusion through the pores is relatively slow compared with the rate of outward migration of calcium.
“Calcium migration is thought to be enhanced in wet conditions (i.e., saturated pores) and at ambient CO2 levels, where CO2 diffusion through the pores is relatively slow compared with the rate of outward migration of calcium73.”
From Spatially resolved nanostructural analysis of disordered phases in carbonated alkali-activated slag (2025) · cites this paper as [73]
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Self-citationEvolution of ettringite in presence of carbonate, and silicate ions
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Efficient CO2 Utilization via a Hybrid Na-CO2 System Based on CO2 Dissolution
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Comparative kinetics study on carbonation of ettringite and meta-ettringite based materials
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Steel corrosion in concrete – Achilles' heel for sustainable concrete?
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Natural carbonation process in cement paste particles in different relative humidities
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Self-citationImpact of the microstructure model on coupled simulation of drying and accelerated carbonation
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Influence of Several Metal lons on the Gelation Activation Energy of Silicon Tetraethoxide
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Atomistic thermodynamics and kinetics of dicalcium silicate dissolution
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Distribution of sulphate and aluminium in hydrated cement pastes
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Surface area changes in C3S paste during the first drying analyzed by 1H NMR relaxometry
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Self-citationIUPAC-NIST Solubility Data Series. 95. Alkaline Earth Carbonates in Aqueous Systems. Part 2. Ca
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Self-citationUnderstanding the Carbonation Phenomenon of C–S–H through Layer Structure Changes and Water Exchange
Uno, T., Saeki, N., Maruyama, I., Suda, Y., Teramoto, A., Kitagaki, R., & Ohkubo, T. (2024) · The Journal of Physical Chemistry C · doi:10.1021/acs.jpcc.4c01714 · Cited by 25 · see citing works
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Cheng, L., & Maruyama, I. (2023) · Journal of Advanced Concrete Technology · doi:10.3151/jact.21.611 · Cited by 9 · see citing works
Self-citationA STUDY ON CALCULATING CO2 UPTAKE DUE TO CARBONATION DURING CONCRETE LIFE-CYCLE
Hyodo, H., Hoshino, S., HIRAO, H., & Nomura, K. (2021) · Cement Science and Concrete Technology · doi:10.14250/cement.74.333 · Cited by 8 · see citing works
A MODEL FOR DISSOLUTION OF CARBON DIOXIDE GAS IN HIGH PH SOLUTION BASED ON CHEMICAL KINETICS
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Saeki, N., Cheng, L., Kurihara, R., & Maruyama, I. (2024) · Cement Science and Concrete Technology · doi:10.14250/cement.77.17 · Cited by 4 · see citing works
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Flagged first, then by citations
2 of the 137 references couldn’t be matched to a known paper.
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Igami, R., Igarashi, G., Aili, A., MINATO, D., Kurihara, R., & Maruyama, I. (2025) · Cement and Concrete Research · doi:10.1016/j.cemconres.2025.107969 · Cited by 52 · see citing works
Self-citationCheng, L., Kurihara, R., Ohkubo, T., Kitagaki, R., Teramoto, A., Suda, Y., & Maruyama, I. (2025) · Cement and Concrete Research · doi:10.1016/j.cemconres.2025.107898 · Cited by 36 · see citing works
Self-citationMa, Z., Wu, Y., Guo, J., Yang, D., & Wu, H. (2026) · Cement and Concrete Composites · doi:10.1016/j.cemconcomp.2026.106723 · Cited by 24 · see citing works
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Accelerated carbonation fronts in cement pastes: Mechanistic insights and simplified modeling
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Self-citationSuda, Y., Ohkubo, T., Teramoto, A., Kitagaki, R., Kurihara, R., & Maruyama, I. (2026) · Cement and Concrete Research · doi:10.1016/j.cemconres.2026.108192 · Cited by 11 · see citing works
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Early carbonation behavior of belite-rich cement: Material foundation and kinetic processes
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Research on the carbonation hardening properties of fully recycled concrete powder compacts
Wang, M., Hu, X., Chen, W., Khaskhoussi, A., Guo, S., & Shi, C. (2026) · Cement and Concrete Composites · doi:10.1016/j.cemconcomp.2026.106556 · Cited by 9 · see citing works
Saito, T., Maruyama, I., Suda, Y., Teramoto, A., Kitagaki, R., & Ohkubo, T. (2025) · ACS Omega · doi:10.1021/acsomega.5c01115 · Cited by 8 · see citing works
Self-citationBui, N. K., Kurihara, R., Noguchi, T., & Maruyama, I. (2025) · Cement and Concrete Composites · doi:10.1016/j.cemconcomp.2025.106392 · Cited by 7 · see citing works
Self-citationSpatially resolved nanostructural analysis of disordered phases in carbonated alkali-activated slag
McCaslin, E. R., James, M. C., Almer, J., Cai, Z., Kenesei, P., Park, J.-S., & White, C. E. (2025) · Nature Communications · doi:10.1038/s41467-025-67179-5 · Cited by 6 · see citing works
“Calciummigrationisthought to beenhanced in wet conditions (i.e., saturated pores) and atambient CO 2 levels, where CO 2 diffusion through the pores is relatively slow compared with the rate of outward migration of calcium 73 .”
Kurihara, R., Cheng, L., Igami, R., Wang, Z., Aili, A., Noto, K., Tanaka, M., Takahashi, H., & Maruyama, I. (2025) · Journal of CO2 Utilization · doi:10.1016/j.jcou.2025.103266 · Cited by 5 · see citing works
Self-citationTomita, S., Yamada, K., Igarashi, G., Hosokawa, Y., & Maruyama, I. (2025) · Journal of Nuclear Materials · doi:10.1016/j.jnucmat.2025.156156 · Cited by 3 · see citing works
Self-citationLi, Y., Xiong, G., Sun, H., Fu, H., Tang, J., Wang, C., & Liu, J. (2025) · Journal of Building Engineering · doi:10.1016/j.jobe.2025.114157 · Cited by 3 · see citing works
Proposal of a new pretreatment of accelerated carbonation for evaluating material potential
Cheng, L., Kurihara, R., Yang, Z., Ohkubo, T., Kitagaki, R., Teramoto, A., Suda, Y., & Maruyama, I. (2026) · Cement and Concrete Composites · doi:10.1016/j.cemconcomp.2026.106633 · Cited by 3 · see citing works
Self-citationJóźwiak–Niedźwiedzka, D., Lisowski, P., Osial, M. E., Brachaczek, A., Alterman, D., & Fantilli, A. P. (2025) · Ceramics · doi:10.3390/ceramics8040140 · Cited by 3 · see citing works
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Self-citationKalpokaitė‐Dičkuvienė, R., Stasiulaitienė, I., Baltušnikas, A., & Yousef, S. (2025) · Materials · doi:10.3390/ma18245636 · Cited by 3 · see citing works
Effects of Relative Humidity on Dissolution and Carbonation Potential of Portlandite
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Self-citationLong-term natural carbonation of blended cements
Rathnakumar, S., Zunino, F., & Scrivener, K. L. (2026) · Cement and Concrete Research · doi:10.1016/j.cemconres.2026.108279 · Cited by 3 · see citing works
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Influence of lime on the evolution of cement mortars carbonation and hydration processes
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In-situ carbonate encapsulation transforms recycled aggregates into carbon-reactive interfaces
Li, C., Qian, X., Qin, Y., Zheng, Y., Mi, T., Shen, P., Hu, C., Wang, F., & Tao, Y. (2026) · Cement and Concrete Composites · doi:10.1016/j.cemconcomp.2026.106753 · Cited by 2 · see citing works
Fully waste-based porous glass-ceramics using incineration bottom ash as self-foaming agent
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Water Adsorption on Portlandite: A Molecular Simulation Study
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Molecular insights into competitive CO2 adsorption between calcium silicate hydrate and portlandite
Zhang, W., Zhang, B., Shi, Y., Guo, X., Li, K., Dang, J., Zhao, J., Zhou, X., & Hou, D. (2026) · Journal of Building Engineering · doi:10.1016/j.jobe.2026.117687
- Authors
- Saeki, N., Kurihara, R., Ohkubo, T., Teramoto, A., Suda, Y., Kitagaki, R., & Maruyama, I.
- Affiliations
- The University of Tokyo (JP)
- Chiba University (JP)
- Hiroshima University (JP)
- University of the Ryukyus (JP)
- Hokkaido University (JP)
- Nagoya University (JP)
- Corresponding author
- Maruyama, Ippei
- Venue
- Cement and Concrete Research
- Publisher
- Elsevier BV
- Published
- 2025-03
- Volume
- 189
- Pages
- 107777
- ISSN
- 0008-8846 (ISSN-L)
- OpenAlex
- W4405887411
- Cited by
- 48
- References
- 137
- Citations by year
- 2026: 30 · 2025: 18
- FWCI
- 8.01
- Type
- journal article
- Language
- en
- Open access
- hybrid
- doi.org
- Licence
- Locations
- Cement and Concrete Research (publishedVersion, cc-by)
- SSRN Electronic Journal (acceptedVersion)
- Funders
- New Energy and Industrial Technology Development Organization (JPNP21023)
- Japan Society for the Promotion of Science (24KJ0825, 23H00203)
- Japan Society for the Promotion of Science London
- Ministry of Education, Culture, Sports, Science and Technology (24UT0002)
- Topics
- Physical Sciences › Engineering › Civil and Structural Engineering › Concrete and Cement Materials Research
- Physical Sciences › Engineering › Civil and Structural Engineering › Concrete Corrosion and Durability
- Physical Sciences › Engineering › Civil and Structural Engineering › Concrete Properties and Behavior
- Keywords
- relative humidity, carbonation kinetics, cement paste, calcium silicate hydrate, calcium hydroxide, metastable phases, phase assemblage, pore solution, CO2 concentration
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