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Shengwen TANG

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Journal of Zhejiang University SCIENCE A 2024 Vol.25 No.2 P.97-115

http://doi.org/10.1631/jzus.A2300476


Stress relaxation properties of calcium silicate hydrate: a molecular dynamics study


Author(s):  Zhicheng GENG, Shengwen TANG, Yang WANG, Hubao A, Zhen HE, Kai WU, Lei WANG

Affiliation(s):  State Key Laboratory of Water Resources Engineering and Management, Wuhan University, Wuhan 430072, China; more

Corresponding email(s):   tangsw@whu.edu.cn

Key Words:  Calcium silicate hydrate (C-S-H), Stress relaxation, Ca/Si ratio, Temperature, Water content, Atomic simulation


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Zhicheng GENG, Shengwen TANG, Yang WANG, Hubao A, Zhen HE, Kai WU, Lei WANG. Stress relaxation properties of calcium silicate hydrate: a molecular dynamics study[J]. Journal of Zhejiang University Science A, 2024, 25(2): 97-115.

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pages="97-115",
year="2024",
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doi="10.1631/jzus.A2300476"
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Abstract: 
The time-dependent viscoelastic response of cement-based materials to applied deformation is far from fully understood at the atomic level. calcium silicate hydrate (C-S-H), the main hydration product of Portland cement, is responsible for the viscoelastic mechanism of cement-based materials. In this study, a molecular model of C-S-H was developed to explain the stress relaxation characteristics of C-S-H at different initial deformation states, ca/Si ratios, temperatures, and water contents, which cannot be accessed experimentally. The stress relaxation of C-S-H occurs regardless of whether it is subjected to initial shear, tensile, or compressive deformation, and shows a heterogeneous characteristic. Water plays a crucial role in the stress relaxation process. A large ca/Si ratio and high temperature reduce the cohesion between the calcium-silicate layer and the interlayer region, and the viscosity of the interlayer region, thereby accelerating the stress relaxation of C-S-H. The effect of the hydrogen bond network and the morphology of C-S-H on the evolution of the stress relaxation characteristics of C-S-H at different water contents was elucidated by nonaffine mean squared displacement. Our results shed light on the stress relaxation characteristics of C-S-H from a microscopic perspective, bridging the gap between the microscopic phenomena and the underlying atomic-level mechanisms.

水化硅酸钙应力松弛特性的分子动力学研究

作者:耿志成1,汤盛文1,2,汪洋1,阿胡宝1,何真1,吴凯2,王磊3
机构:1武汉大学,水资源工程与调度全国重点实验室,中国武汉,430072;2同济大学,先进土木工程材料教育部重点实验室,中国上海,200092;3西安建筑科技大学,材料科学与工程学院,中国西安,710055
目的:水化硅酸钙(C-S-H)是波特兰水泥的主要水化产物,是影响水泥基材料粘弹性机制的主要成分之一。然而,人们还未能在原子层面上完全理解水泥基材料在外加变形作用下随时间变化的粘弹性响应。本文旨在通过建立不同钙硅比的C-S-H模型,以分子动力学模拟的方式系统研究不同因素对水化硅酸钙应力松弛性能的影响。
创新点:1.基于分子动力学模拟,获得C-S-H的应力松弛特性;2.研究应变状态、钙硅比和内部水含量对C-S-H应力松弛的影响,揭示其在应力松弛过程中所涉及的内部结构及能量变化。
方法:1.通过各原子基团的均方位移在应力松弛过程中考虑C-S-H层间区域的粘度变化;2.基于时间相关函数,在不同应变状态、钙硅比以及温度的条件下研究C-S-H层间区域涉及到的化学键断裂与重组;3.阐明氢键网络和C-S-H形态对不同含水量下C-S-H应力松弛特性演变的影响。
结论:1.在不同的初始变形条件下,C-S-H应力松弛响应均会发生,并显示出非均质特征;2.钙硅比的增大以及温度的提高会导致水分子、羟基和层间钙原子的运动加快,从而引起C-S-H层间区域的粘度降低,进而导致C-S-H的初始应力及残余应力降低;3.由于水分子会影响C-S-H的形貌以及层间氢键网络,所以C-S-H在不同水含量时展现出不同的应力松弛特性。

关键词:水化硅酸钙;应力松弛;钙硅比;温度;水含量;原子模拟

Darkslateblue:Affiliate; Royal Blue:Author; Turquoise:Article

Reference

[1]Abdolhosseini QomiMJ, KrakowiakKJ, BauchyM, et al., 2014. Combinatorial molecular optimization of cement hydrates. Nature Communications, 5:4960.

[2]AlizadehR, BeaudoinJJ, RakiL, 2010. Viscoelastic nature of calcium silicate hydrate. Cement and Concrete Composites, 32(5):369-376.

[3]AllenAJ, ThomasJJ, JenningsHM, 2007. Composition and density of nanoscale calcium‍–‍silicate‍–‍hydrate in cement. Nature Materials, 6(4):311-316.

[4]ArayroJ, DufresneA, ZhouTT, et al., 2018. Thermodynamics, kinetics, and mechanics of cesium sorption in cement paste: a multiscale assessment. Physical Review Materials, 2(5):053608.

[5]AtutisM, ValivonisJ, AtutisE, 2018. Experimental study of concrete beams prestressed with basalt fiber reinforced polymers. Part II: stress relaxation phenomenon. Composite Structures, 202:344-354.

[6]BazantZP, ChernJC, 1985. Concrete creep at variable humidity: constitutive law and mechanism. Materials and Structures, 18(1):1-20.

[7]BažantZP, HauggaardAB, BawejaS, et al., 1997. Microprestress-solidification theory for concrete creep. I: aging and drying effects. Journal of Engineering Mechanics, 123(11):1188-1194.

[8]BeushausenH, MasukuC, MoyoP, 2012. Relaxation characteristics of cement mortar subjected to tensile strain. Materials and Structures, 45(8):1181-1188.

[9]BrooksJJ, NevilleAM, 1976. Relaxation of stress in concrete and its relation to creep. Journal Proceedings, 73(4):‍227-232.

[10]ChenJ, FangL, ChenHQ, et al., 2022. The loading speed facilitating stress relaxation behaviors of surface-modified silicon: a molecular dynamics study. Journal of Molecular Modeling, 28(6):160.

[11]ChenJK, QianC, 2017. Loading history dependence of retardation time of calcium-silicate-hydrate. Construction and Building Materials, 147:558-565.

[12]CiarellaS, SciortinoF, EllenbroekWG, 2018. Dynamics of vitrimers: defects as a highway to stress relaxation. Physical Review Letters, 121(5):058003.

[13]ConstantinidesG, UlmFJ, 2004. The effect of two types of C-S-H on the elasticity of cement-based materials: results from nanoindentation and micromechanical modeling. Cement and Concrete Research, 34(1):67-80.

[14]ConstantinidesG, UlmFJ, 2007. The nanogranular nature of C-S-H. Journal of the Mechanics and Physics of Solids, 55(1):64-90.

[15]CuestaA, SantacruzI, de la TorreAG, et al., 2021. Local structure and Ca/Si ratio in C-S-H gels from hydration of blends of tricalcium silicate and silica fume. Cement and Concrete Research, 143:106405.

[16]CyganRT, LiangJJ, KalinichevAG, 2004. Molecular models of hydroxide, oxyhydroxide, and clay phases and the development of a general force field. The Journal of Physical Chemistry B, 108(4):1255-1266.

[17]DingH, ChenJK, 2019. Research on the resistivity attenuation law of cementitious conductive composites induced by stress relaxation. Construction and Building Materials, 206:347-354.

[18]DuHJ, PangSD, 2021. Long-term influence of nanosilica on the microstructures, strength, and durability of high-volume fly ash mortar. Journal of Materials in Civil Engineering, 33(8):04021185.

[19]FalkML, LangerJS, 1998. Dynamics of viscoplastic deformation in amorphous solids. Physical Review E, 57(6):7192-7205.

[20]FangGH, ZhangMZ, 2020. Multiscale micromechanical analysis of alkali-activated fly ash-slag paste. Cement and Concrete Research, 135:106141.

[21]FeldmanRF, 1972. Mechanism of creep of hydrated Portland cement paste. Cement and Concrete Research, 2(5):‍521-540.

[22]FengD, LiXF, WangXZ, et al., 2018. Capillary filling under nanoconfinement: the relationship between effective viscosity and water-wall interactions. International Journal of Heat and Mass Transfer, 118:900-910.

[23]Frech-BaronetJ, SorelliL, CharronJP, 2017. New evidences on the effect of the internal relative humidity on the creep and relaxation behaviour of a cement paste by micro-indentation techniques. Cement and Concrete Research, 91:39-51.

[24]FuQ, XieYJ, LongGC, et al., 2015. Temperature sensitivity and model of stress relaxation properties of cement and asphalt mortar. Construction and Building Materials, 84:1-11.

[25]GallucciE, ZhangX, ScrivenerKL, 2013. Effect of temperature on the microstructure of calcium silicate hydrate (C-S-H). Cement and Concrete Research, 53:185-195.

[26]GaoY, ZhangJ, HanP, 2013. Determination of stress relaxation parameters of concrete in tension at early-age by ring test. Construction and Building Materials, 41:152-164.

[27]GiorlaAB, DunantCF, 2018. Microstructural effects in the simulation of creep of concrete. Cement and Concrete Research, 105:44-53.

[28]GowersRJ, CarboneP, 2015. A multiscale approach to model hydrogen bonding: the case of polyamide. The Journal of Chemical Physics, 142(22):224907.

[29]HanGZ, FangZK, ChenMD, 2010. Modified Eyring viscosity equation and calculation of activation energy based on the liquid quasi-lattice model. Science China Physics, Mechanics and Astronomy, 53(10):1853-1860.

[30]HouDS, MaHY, YuZ, et al., 2014a. Calcium silicate hydrate from dry to saturated state: structure, dynamics and mechanical properties. Acta Materialia, 67:81-94.

[31]HouDS, ZhuY, LuYY, et al., 2014b. Mechanical properties of calcium silicate hydrate (C-S-H) at nano-scale: a molecular dynamics study. Materials Chemistry and Physics, 146(3):503-511.

[32]HouDS, ZhaoTJ, MaHY, et al., 2015a. Reactive molecular simulation on water confined in the nanopores of the calcium silicate hydrate gel: structure, reactivity, and mechanical properties. The Journal of Physical Chemistry C, 119(3):1346-1358.

[33]HouDS, ZhangJR, LiZJ, et al., 2015b. Uniaxial tension study of calcium silicate hydrate (C-S-H): structure, dynamics and mechanical properties. Materials and Structures, 48(11):3811-3824.

[34]HouDS, LiZJ, ZhaoTJ, et al., 2015c. Water transport in the nano-pore of the calcium silicate phase: reactivity, structure and dynamics. Physical Chemistry Chemical Physics, 17(2):1411-1423.

[35]HouDS, YuJ, JinZQ, et al., 2018a. Molecular dynamics study on calcium silicate hydrate subjected to tension loading and water attack: structural evolution, dynamics degradation and reactivity mechanism. Physical Chemistry Chemical Physics, 20(16):11130-11144.

[36]HouDS, JiaYT, YuJ, et al., 2018b. Transport properties of sulfate and chloride ions confined between calcium silicate hydrate surfaces: a molecular dynamics study. The Journal of Physical Chemistry C, 122(49):28021-28032.

[37]JanaR, PastewkaL, 2019. Correlations of non-affine displacements in metallic glasses through the yield transition. Journal of Physics: Materials, 2(4):045006.

[38]JenningsHM, 2004. Colloid model of C-S-H and implications to the problem of creep and shrinkage. Materials and Structures Aims, 37(1):59-70.

[39]KaiMF, ZhangLW, LiewKM, 2021. New insights into creep characteristics of calcium silicate hydrates at molecular level. Cement and Concrete Research, 142:106366.

[40]LiB, LiN, BrouwersHJH, et al., 2020. Understanding hydrogen bonding in calcium silicate hydrate combining solid-state NMR and first principle calculations. Construction and Building Materials, 233:117347.

[41]LiJ, YuQJ, HuangHL, et al., 2019. Effects of Ca/Si ratio, aluminum and magnesium on the carbonation behavior of calcium silicate hydrate. Materials, 12(8):1268.

[42]LiX, GrasleyZC, GarbocziEJ, et al., 2015. Modeling the apparent and intrinsic viscoelastic relaxation of hydrating cement paste. Cement and Concrete Composites, 55:‍322-330.

[43]LiXD, GrasleyZC, BullardJW, et al., 2018. Creep and relaxation of cement paste caused by stress-induced dissolution of hydrated solid components. Journal of the American Ceramic Society, 101(9):4237-4255.

[44]LiZM, ZhangSZ, LiangXH, et al., 2020. Cracking potential of alkali-activated slag and fly ash concrete subjected to restrained autogenous shrinkage. Cement and Concrete Composites, 114:103767.

[45]LiangCY, ZhengQ, JiangJY, et al., 2022. Calcium silicate hydrate colloid at different humidities: microstructure, deformation mechanism, and mechanical properties. Acta Materialia, 228:117740.

[46]LiuWH, ZhangLW, LiewKM, 2020. Modeling of crack bridging and failure in heterogeneous composite materials: a damage-plastic multiphase model. Journal of the Mechanics and Physics of Solids, 143:104072.

[47]LothenbachB, ScrivenerK, HootonRD, 2011. Supplementary cementitious materials. Cement and Concrete Research, 41(12):1244-1256.

[48]ManzanoH, PellenqRJM, UlmFJ, et al., 2012. Hydration of calcium oxide surface predicted by reactive force field molecular dynamics. Langmuir, 28(9):4187-4197.

[49]ManzanoH, MasoeroE, Lopez-ArbeloaI, et al., 2013. Shear deformations in calcium silicate hydrates. Soft Matter, 9(30):7333-7341.

[50]MaruyamaI, IgarashiG, NishiokaY, 2015. Bimodal behavior of C-S-H interpreted from short-term length change and water vapor sorption isotherms of hardened cement paste. Cement and Concrete Research, 73:158-168.

[51]MasoumiS, ZareS, ValipourH, et al., 2019. Effective interactions between calcium‍-silicate-hydrate nanolayers. The Journal of Physical Chemistry C, 123(8):4755-4766.

[52]MorshedifardA, MasoumiS, Abdolhosseini QomiMJ, 2018. Nanoscale origins of creep in calcium silicate hydrates. Nature Communications, 9(1):1785.

[53]MortazaviB, JavvajiB, ShojaeiF, et al., 2021a. Exceptional piezoelectricity, high thermal conductivity and stiffness and promising photocatalysis in two-dimensional MoSi2N4 family confirmed by first-principles. Nano Energy, 82:105716.

[54]MortazaviB, SilaniM, PodryabinkinEV, et al., 2021b. First-principles multiscale modeling of mechanical properties in graphene/borophene heterostructures empowered by machine-learning interatomic potentials. Advanced Materials, 33(35):2102807.

[55]PellenqRJM, KushimaA, ShahsavariR, et al., 2009. A realistic molecular model of cement hydrates. Proceedings of the National Academy of Sciences of the United States of America, 106(38):16102-16107.

[56]PitmanMC, van DuinACT, 2012. Dynamics of confined reactive water in smectite clay‍–‍zeolite composites. Journal of the American Chemical Society, 134(6):3042-3053.

[57]PriezjevNV, 2017. Collective nonaffine displacements in amorphous materials during large-amplitude oscillatory shear. Physical Review E, 95(2):023002.

[58]RichardsonIG, 1999. The nature of C-S-H in hardened cements. Cement and Concrete Research, 29(8):1131-1147.

[59]RongH, DongW, ZhaoXY, et al., 2021. Investigation on multi-cracks initiation and propagation of fiber reinforced concrete in restrained shrinkage ring tests. Theoretical and Applied Fracture Mechanics, 111:102856.

[60]RossiP, 1997. Strain rate effects in concrete structures: the LCPC experience. Materials and Structures, 30(1):54-62.

[61]ScrivenerKL, KirkpatrickRJ, 2008. Innovation in use and research on cementitious material. Cement and Concrete Research, 38(2):128-136.

[62]ShahsavariR, PellenqRJM, UlmFJ, 2011. Empirical force fields for complex hydrated calcio-silicate layered materials. Physical Chemistry Chemical Physics, 13(3):‍1002-1011.

[63]ShimizuF, OgataS, LiJ, 2007. Theory of shear banding in metallic glasses and molecular dynamics calculations. Materials Transactions, 48(11):2923-2927.

[64]ShishegaranA, KhaliliMR, KaramiB, et al., 2020. Computational predictions for estimating the maximum deflection of reinforced concrete panels subjected to the blast load. International Journal of Impact Engineering, 139:103527.

[65]TalebiH, SilaniM, BordasSPA, et al., 2014. A computational library for multiscale modeling of material failure. Computational Mechanics, 53(5):1047-1071.

[66]TamtsiaBT, BeaudoinJJ, 2000. Basic creep of hardened cement paste: a re-examination of the role of water. Cement and Concrete Research, 30(9):1465-1475.

[67]TangC, WongCH, 2015. Effect of atomic-level stresses on local dynamic and mechanical properties in CuxZr100-x metallic glasses: a molecular dynamics study. Intermetallics, 58:50-55.

[68]TianHW, StephanD, LothenbachB, et al., 2021. Influence of foreign ions on calcium silicate hydrate under hydrothermal conditions: a review. Construction and Building Materials, 301:124071.

[69]ToddBD, DaivisPJ, 2017. Nonequilibrium Molecular Dynamics: Theory, Algorithms and Applications. Cambridge University Press, Cambridge, UK.

[70]VandewalleL, NemegeerD, BalazsL, et al., 2002. Design of steel fibre reinforced concrete using the σ‍-‍w method: principles and applications. Materials and Structures, 35:262-278.

[71]VenkovicN, SorelliL, MartirenaF, 2014. Nanoindentation study of calcium silicate hydrates in concrete produced with effective microorganisms-based bioplasticizer. Cement and Concrete Composites, 49:127-139.

[72]WangJW, KalinichevAG, KirkpatrickRJ, 2004. Molecular modeling of water structure in nano-pores between brucite (001) surfaces. Geochimica et Cosmochimica Acta, 68(16):3351-3365.

[73]WangXF, BaoYW, LiuXG, et al., 2015. The stress relaxation of cement clinkers under high temperature. Frontiers of Mechanical Engineering, 10(4):413-417.

[74]WangZP, ChenYT, XuLL, et al., 2022. Insight into the local C-S-H structure and its evolution mechanism controlled by curing regime and Ca/Si ratio. Construction and Building Materials, 333:127388.

[75]YangXS, WangYJ, WangGY, et al., 2016. Time, stress, and temperature-dependent deformation in nanostructured copper: stress relaxation tests and simulations. Acta Materialia, 108:252-263.

[76]YoussefM, PellenqRJM, YildizB, 2011. Glassy nature of water in an ultraconfining disordered material: the case of calcium‍–‍silicate‍–‍hydrate. Journal of the American Chemical Society, 133(8):2499-2510.

[77]ZhangMZ, YeG, van BreugelK, 2011. Microstructure-based modeling of water diffusivity in cement paste. Construction and Building Materials, 25(4):2046-2052.

[78]ZhangT, QinWZ, 2006. Tensile creep due to restraining stresses in high-strength concrete at early ages. Cement and Concrete Research, 36(3):584-591.

[79]ZhangY, ZhouQ, JuJW, et al., 2021. New insights into the mechanism governing the elasticity of calcium silicate hydrate gels exposed to high temperature: a molecular dynamics study. Cement and Concrete Research, 141:106333.

[80]ZhengQ, JiangJY, LiXL, et al., 2021. In situ TEM observation of calcium silicate hydrate nanostructure at high temperatures. Cement and Concrete Research, 149:106579.

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