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基于分子动力学模拟的过硫磷石膏矿渣水泥组成设计

徐方 李恒 孙涛 水中和 丁超

徐方, 李恒, 孙涛, 等. 基于分子动力学模拟的过硫磷石膏矿渣水泥组成设计[J]. 复合材料学报, 2022, 39(6): 2821-2828. doi: 10.13801/j.cnki.fhclxb.20210816.005
引用本文: 徐方, 李恒, 孙涛, 等. 基于分子动力学模拟的过硫磷石膏矿渣水泥组成设计[J]. 复合材料学报, 2022, 39(6): 2821-2828. doi: 10.13801/j.cnki.fhclxb.20210816.005
XU Fang, LI Heng, SUN Tao, et al. Composition design of excess-sulfate phosphogypsum slag cement based on molecular dynamics simulation[J]. Acta Materiae Compositae Sinica, 2022, 39(6): 2821-2828. doi: 10.13801/j.cnki.fhclxb.20210816.005
Citation: XU Fang, LI Heng, SUN Tao, et al. Composition design of excess-sulfate phosphogypsum slag cement based on molecular dynamics simulation[J]. Acta Materiae Compositae Sinica, 2022, 39(6): 2821-2828. doi: 10.13801/j.cnki.fhclxb.20210816.005

基于分子动力学模拟的过硫磷石膏矿渣水泥组成设计

doi: 10.13801/j.cnki.fhclxb.20210816.005
基金项目: 2020年度中山市第三批科技发展专项资金资助项目(2020-18);中山市武汉理工大学先进工程技术研究院科研项目(WUT202011);湖北省交通运输厅科技项目(2020-2-1-10)
详细信息
    通讯作者:

    孙涛,博士,副研究员,研究方向为水泥与混凝土  E-mail:sunt@whut.edu.cn

  • 中图分类号: TU528

Composition design of excess-sulfate phosphogypsum slag cement based on molecular dynamics simulation

  • 摘要: 原材料化学成分的组成设计是过硫磷石膏矿渣水泥(PPSC)水化反应与力学强度形成的基础,室内试验与分子动力学模拟(MD)为PPSC原材料的化学组成提供了多尺度调控设计依据。利用Materials Studio(MS)软件建立PPSC结构模型,采用MD与XRD等手段研究了化学成分摩尔比对PPSC抗压强度的影响规律。结果表明:随着CaO/SO3摩尔比的增加和SiO2/Al2O3的降低,PPSC的抗压强度呈增长趋势,当SiO2/Al2O3摩尔比为3.5~3.7、CaO/SO3摩尔比为1.8~2.0时,PPSC的抗压强度较高。分子动力学对PPSC孔结构的模拟结果与抗压强度试验结果规律相反,证明了模拟结果的可靠性。在原子尺度上,分子动力学模拟表明O、Ca、Al及S原子表现出较高的扩散能力,在碱性环境下,硫酸盐激发作用使S=O、Al—O及O=O键长增大而结构失稳水解,生成较多对强度起促进作用的钙矾石。通过调控原材料SiO2/Al2O3摩尔比和CaO/SO3摩尔比可使PPSC形成更加稳定的内部结构。化学成分摩尔比设计及分子动力学模拟方法对PPSC的组成设计和应用推广具有重要意义。

     

  • 图  1  过硫磷石膏矿渣水泥(PPSC)制备流程图

    Figure  1.  Flow chart of preparation of excess-sulfate phosphogypsum slag cement (PPSC)

    图  2  PPSC抗压强度

    Figure  2.  Compressive strength of PPSC

    图  3  PPSC模型基本单元 (a) 和最终模型 (b)

    Figure  3.  Basic unit of PPSC model (a) and final models (b) of PPSC

    图  4  PPSC的XRD图谱

    Figure  4.  XRD pattens of PPSC

    图  5  PPSC模型总径向分布函数

    Figure  5.  Total radial distribution function of PPSC models

    图  6  PPSC模型各原子键的径向分布函数

    Figure  6.  Radial distribution function of each atomic bond in PPSC models

    图  7  PPSC模型原子表面积和孔结构分布

    Figure  7.  Distribution of atomic surface and pore structure of PPSC models

    图  8  PPSC模型原子表面积和孔结构体积

    Figure  8.  Atomic surface area and pore volume of PPSC models

    图  9  PPSC模型中各原子扩散系数

    Figure  9.  Diffusion coefficient of each atom in PPSC models

    表  1  磷石膏(PG)、水泥和矿粉(GGBS)的化学组成

    Table  1.   Chemical compositions of phosphogypsum (PG), cement and granulated blast furnace slag powder (GGBS) wt%

    CompositionSiO2Al2O3SO3CaOMgOFe2O3TiO2P2O5Loss
    PG 2.26 0.40 49.38 38.89 0.06 0.38 0.35 0.43 7.71
    Cement 19.14 5.11 4.42 59.03 1.96 3.74 0.33 5.52
    GGBS 34.74 16.45 3.62 33.55 6.42 1.77 1.75 1.64
    下载: 导出CSV

    表  2  PPSC配合比设计

    Table  2.   Mix design of PPSC

    Sample
    Mass fraction/wt%Molar ratio
    PGGGBSCementSiO2/Al2O3CaO/SO3
    P70G25C5 70 25 5 3.5 1.6
    P60G35C5 60 35 5 3.5 1.8
    P50G45C5 50 45 5 3.5 2.0
    P70G20C10 70 20 10 3.7 1.6
    P60G30C10 60 30 10 3.7 1.8
    P50G40C10 50 40 10 3.7 2.0
    P70G15C15 70 15 15 3.9 1.6
    P60G25C15 60 25 15 3.9 1.8
    P50G35C15 50 35 15 3.9 2.0
    Notes: P—Phosphogypsum; G—Granulated blast furnace slag powder; C—Cement. The number after the letter indicates the percentage content; Abbreviations in this table do not contradict other abbreviations in this paper.
    下载: 导出CSV

    表  3  PPSC分子动力学模型中基本单元个数

    Table  3.   Number of basic units in PPSC molecular dynamics models

    SampleSi/AlCa/SCaSO3H2OSiAlO7Si2AlO10
    P50G45C5 1.75 2.0 86 43 86 5 15
    P70G20C10 1.85 1.6 180 112 224 3 17
    P50G40C10 1.85 2.0 92 46 92 3 17
    Note: Si/Al and Ca/S—Ratio of atomic amount.
    下载: 导出CSV

    表  4  PPSC模型中各原子键键长

    Table  4.   Bond length of each atomic bond in PPSC models nm

    SampleSi/AlCa/SCa—OAl—OSi—OS=OH—OO=O
    P50G45C5 1.75 2.0 0.221 0.167 0.165 0.163 0.095 0.271
    P70G20C10 1.85 1.6 0.221 0.169 0.167 0.143 0.097 0.247
    P50G40C10 1.85 2.0 0.221 0.219 0.167 0.163 0.097 0.271
    Reference 0.251 0.163 0.159 0.097 0.269-0.271
    下载: 导出CSV
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出版历程
  • 收稿日期:  2021-05-17
  • 修回日期:  2021-07-29
  • 录用日期:  2021-07-30
  • 网络出版日期:  2021-08-17
  • 刊出日期:  2022-06-01

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