Effect of Calcium Silicon Ratio on Sintering Behavior and Carbon Sequestration Capacity of Calcium Silicate Mineral Phase

doi:10.16552/j.cnki.issn1001-1625.2024.0797

Abstract

Abstract: Calcium silicate carbonatable binder is an important direction to realize the green and sustainable development of building materials industry. In order to study the effect of calcium silicon ratio (n(CaO)∶n(SiO₂), molar ratio) on the composition of calcium silicate mineral phase and their carbon sequestration capabilities, calcium silicate carbonatable binders were synthesized with controlled calcium silicon ratio (n(CaO)∶n(SiO₂)=1.8~2.2). Techniques such as t-pH, XRD, TGA, and SEM were employed to examine the evolution of phase composition, carbonization hardening process, CO₂ uptakes and carbonization products of calcium silicate carbonatable binders. The results indicate that the content of γ-dicalcium silicate (Ca₂SiO₄, γ-C₂S) initially increases and subsequently decreases as the calcium silicon ratio rises. When the calcium silicon ratio is no higher than 2.0, the content of rankinite (Ca₃Si₂O₇, C₃S₂) gradually increases with the decreasing of calcium silicon ratio. When the calcium silicon ratio is higher than 2.0, the content of β-dicalcium silicate (Ca₂SiO₄, β-C₂S) progressively increases with the increasing of calcium silicon ratio. The reaction of carbonization for 0.5 h is intense, and the compressive strength initial increases and subsequent decreases as the calcium silicon ratio increases. The reaction produces calcite, aragonite and vaterite. With the content of C₃S₂ and γ-C₂S decreasing significantly, and the calcite content remains largely unchanged even when the carbonization reaction is extended to 24 h. C₃S₂ decelerates the early reaction of binder, but a more sustained carbonization reaction and a greater variety of carbonization products can enhance its subsequent compressive strength. The compressive strength and CO₂ uptakes after carbonization for 24 h reach 129.76 MPa and 18.57%, respectively.

Key words: calcium silicon ratio, calcium silicate, sintering behavior, carbon sequestration capacity, compressive strength

CLC Number:

TQ172

CHEN Ping, LI Fangbin, XIANG Weiheng, HU Cheng, LIU Jun, WANG Qijie. Effect of Calcium Silicon Ratio on Sintering Behavior and Carbon Sequestration Capacity of Calcium Silicate Mineral Phase[J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2025, 44(1): 297-304.

References

[1] JIANG K, ASHWORTH P. The development of carbon capture utilization and storage (CCUS) research in China: a bibliometric perspective[J]. Renewable and Sustainable Energy Reviews, 2021, 138: 110521.
[2] 吴胜坤, 黄天勇, 谢岩, 等. 二氧化碳矿化养护水泥基材料研究进展[J]. 硅酸盐通报, 2023, 42(6): 1897-1911.
WU S K, HUANG T Y, XIE Y, et al. Review on CO₂ mineral carbonation-cured cement-based materials[J]. Bulletin of the Chinese Ceramic Society, 2023, 42(6): 1897-1911 (in Chinese).
[3] LIU Z C, LV C Y, WANG F Z, et al. Recent advances in carbonatable binders[J]. Cement and Concrete Research, 2023, 173: 107286.
[4] 刘志超, 王发洲, 胡曙光. 固碳胶凝材料研究进展[J]. 硅酸盐学报, 2023, 51(5): 1234-1245.
LIU Z C, WANG F Z, HU S G. Development of carbonatable binders: a short review[J]. Journal of the Chinese Ceramic Society, 2023, 51(5): 1234-1245 (in Chinese).
[5] ASHRAF W, OLEK J. Carbonation behavior of hydraulic and non-hydraulic calcium silicates: potential of utilizing low-lime calcium silicates in cement-based materials[J]. Journal of Materials Science, 2016, 51(13): 6173-6191.
[6] ASHRAF W, OLEK J. Elucidating the accelerated carbonation products of calcium silicates using multi-technique approach[J]. Journal of CO₂ Utilization, 2018, 23: 61-74.
[7] MU Y D, LIU Z C, WANG F Z. Comparative study on the carbonation-activated calcium silicates as sustainable binders: reactivity, mechanical performance, and microstructure[J]. ACS Sustainable Chemistry & Engineering, 2019, 7(7): 7058-7070.
[8] JIANG T, CUI K, CHANG J. Development of low-carbon cement: carbonation of compounded C₂S by β-C₂S and γ-C₂S[J]. Cement and Concrete Composites, 2023, 139: 105071.
[9] CHANG J, JIANG T, CUI K. Influence on compressive strength and CO₂ capture after accelerated carbonation of combination β-C₂S with γ-C₂S[J]. Construction and Building Materials, 2021, 312: 125359.
[10] 黎帅, 周凤娇, 谭新宇, 等. 二氧化碳浓度对低钙固碳胶凝材料性能影响及机理研究[J]. 硅酸盐通报, 2023, 42(9): 3109-3116.
LI S, ZHOU F J, TAN X Y, et al. Effect of carbon dioxide concentration on performance of low-calcium carbon sequestration cementitious materials and its mechanism[J]. Bulletin of the Chinese Ceramic Society, 2023, 42(9): 3109-3116 (in Chinese).
[11] 侯贵华, 卢豹, 郜效娇, 等. 新型低钙水泥的制备及其碳化硬化过程[J]. 硅酸盐学报, 2016, 44(2): 286-291.
HOU G H, LU B, GAO X J, et al. Preparation and carbonation-hardening process of low-calcium cement composition[J]. Journal of the Chinese Ceramic Society, 2016, 44(2): 286-291 (in Chinese).
[12] KOUTNÍK P. Preparation of β-belite using liquid alkali silicates[J]. Materiales de Construcción, 2017, 67(328): 140.
[13] 管学茂, 邱满, 李海艳, 等. 自粉化低钙水泥的制备方法及其碳化硬化性能[J]. 建筑材料学报, 2018, 21(5): 775-779+785.
GUAN X M, QIU M, LI H Y, et al. Preparation of self-pulverized low calcium cement and its carbonation-hardening properties[J]. Journal of Building Materials, 2018, 21(5): 775-779+785 (in Chinese).
[14] 田键. 硅酸盐晶体化学[M]. 武汉: 武汉大学出版社, 2010: 166.
TIAN J. Crystal chemistry of silicate[M]. Wuhan: Wuhan University Press, 2010: 166 (in Chinese).
[15] LIU S H, RONG P J, ZHANG C, et al. Preparation and carbonation hardening of low calcium CO₂ sequestration materials from waste concrete powder and calcium carbide slag[J]. Cement and Concrete Composites, 2023, 141: 105151.
[16] CHANG J, FANG Y F, SHANG X P. The role of β-C₂S and γ-C₂S in carbon capture and strength development[J]. Materials and Structures, 2016, 49(10): 4417-4424.
[17] 穆元冬. 硅酸钙矿物碳酸化固化机理及其材料性能提升机制研究[D]. 武汉: 武汉理工大学, 2019: 33-34.
MU Y D. Study on carbonation curing mechanism of calcium silicate mineral and its material performance improvement mechanism[D]. Wuhan: Wuhan University of Technology, 2019: 33-34 (in Chinese).
[18] LIN S Q, CHEN P, XIANG W H, et al. Exploring the effect of moisture on CO₂ diffusion and particle cementation in carbonated steel slag[J]. Applied Sciences, 2024, 14(9): 3631.
[19] KOUMPOURI D, ANGELOPOULOS G N. Effect of boron waste and boric acid addition on the production of low energy belite cement[J]. Cement and Concrete Composites, 2016, 68: 1-8.
[20] FU X X, GUERINI A, ZAMPINI D, et al. Storing CO₂ while strengthening concrete by carbonating its cement in suspension[J]. Communications Materials, 2024, 5: 109.
[21] MU Y D, LIU Z C, WANG F Z, et al. Carbonation characteristics of γ-dicalcium silicate for low-carbon building material[J]. Construction and Building Materials, 2018, 177: 322-331.
[22] 赵思雪, 刘志超, 王发洲. 超高强碳矿化材料的设计与制备[J]. 硅酸盐学报, 2023, 51(9): 2128-2137.
ZHAO S X, LIU Z C, WANG F Z. Design and preparation of ultra-high strength CO₂ solidified carbonate materials[J]. Journal of the Chinese Ceramic Society, 2023, 51(9): 2128-2137 (in Chinese).