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A molecular dynamics study of calcium silicate hydrates-aggregate interfacial interactions and influence of moisture

水化硅酸钙-集料界面交互作用及湿度影响的分子动力学研究

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Abstract

The interface properties between hydrated cement paste (hcp) and aggregates largely determine the various performances of concrete. In this work, molecular dynamics simulations were employed to explore the atomistic interaction mechanisms between the commonly used aggregate phase calcite/silica and calcium silicate hydrates (C-S-H), as well as the effect of moisture. The results suggest that the C-S-H/calcite interface is relatively strong and stable under both dry and moist conditions, which is caused by the high-strength interfacial connections formed between calcium ions from calcite and high-polarity non-bridging oxygen atoms from the C-S-H surface. Silica can be also adsorbed on the dry C-S-H surface by the H-bonds; however, the presence of water molecules on the interface may substantially decrease the affinities. Furthermore, the dynamics interface separation tests of C-S-H/aggregates were also implemented by molecular dynamics. The shape of the calculated stress-separation distance curves obeys the quasi-static cohesive law obtained experimentally. The moisture conditions and strain rates were found to affect the separation process of C-S-H/silica. A wetter interface and smaller loading rate may lead to a lower adhesion strength. The mechanisms interpreted here may shed new lights on the understandings of hcp/aggregate interactions at a nano-length scale and creation of high performance cementitious materials.

摘要

水泥水化浆体与集料的界面性质在很大程度上决定了混凝土的各项性能。 本研究利用分子动力学模拟探讨了常用的集料相碳酸钙/二氧化硅与水化硅酸钙(C-S-H)之间的界面相互作用机制, 以及湿度对界面性质的影响。 结果表明, 无论在干或湿条件下, C-S-H/碳酸钙界面都具有较强的稳定性。 这是由于碳酸钙中钙离子与 C-S-H 表面的高极性非桥氧原子具有高强度化学连接的原因。 二氧化硅则通过氢键作用吸附于干燥的 C-S-H 表面,但界面上水分子的存在会大大降低界面亲和度。 此外, 还利用分子动力学进行了 C-S-H/集料界面分离的动态模拟, 计算结果趋势符合准静态黏聚法则。 而润湿度和拉伸速率对 C-S-H/二氧化硅的分离过程有较为明显的影响, 较湿润的界面和较小的加载速率均有可能导致黏聚力降低。 本研究可为纳米尺度下理解浆体/集料相互作用以及高性能水泥基材料的研制提供新的思路。

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Authors and Affiliations

  1. School of Materials Science and Engineering, Southeast University, Nanjing, 211189, China

    Yang Zhou  (周扬), Ze-chuan Peng  (彭泽川), Jia-le Huang  (黄家乐) & Chang-wen Miao  (缪昌文)

  2. State Key Laboratory of High Performance Civil Engineering Materials, Jiangsu Research Institute of Building Science Co., Nanjing, 211103, China

    Yang Zhou  (周扬), Ze-chuan Peng  (彭泽川), Jia-le Huang  (黄家乐) & Chang-wen Miao  (缪昌文)

  3. School of Transportation, Southeast University, Nanjing, 211189, China

    Tao Ma  (马涛) & Xiao-ming Huang  (黄晓明)

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Contributions

The overarching research goals were developed by ZHOU Yang, PENG Ze-chuan, HUANG Jia-le, MA Tao, HUANG Xiao-ming and MIAO Chang-wen. ZHOU Yang, MA Tao, HUANG Xiao-ming and MIAO Chang-wen contributed to the conception of the study. PENG Ze-chuan and HUANG Jia-le designed and performed the simulations. ZHOU Yang and HUANG Jia-le performed the data analysis and wrote the manuscript. ZHOU Yang and HUANG Jia-le replied to reviewers’ comments and revised the final version.

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Correspondence to Jia-le Huang  (黄家乐).

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Conflict of interest

ZHOU Yang, PENG Ze-chuan, HUANG Jia-le, MA Tao, HUANG Xiao-ming and MIAO Chang-wen declare that they have no conflict of interest.

Foundation item

Projects(6512009004A, 51908119, U1706222) supported by the National Natural Science Foundation of China; Project(BK20190367) supported by the Natural Science Foundation of Jiangsu Province, China

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Zhou, Y., Peng, Zc., Huang, Jl. et al. A molecular dynamics study of calcium silicate hydrates-aggregate interfacial interactions and influence of moisture. J. Cent. South Univ. 28, 16–28 (2021). https://doi.org/10.1007/s11771-021-4582-4

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