介孔尺度及结构对混合硝酸盐热输运特性的影响

何卓亚; 杨启容; 李昭莹; 毛蕊; 王力伟; 闫晨宣

doi:10.7498/aps.71.20211276

摘要

采用分子动力学方法模拟介孔尺度和结构对混合硝酸盐热输运特性的影响. 使用Material Studio软件分别建立不同尺度、两种结构的混合硝酸盐模型以及达到共晶状态的不同比例的NaNO₃-KNO₃模型, 通过对模型进行运算并整理计算结果, 对纳米尺度下混合硝酸盐热输运特性的微观机理进行分析. 结果表明: 太阳盐的相变温度随着纳米孔尺度的增大呈现先增加后减小的趋势, 最终与宏观尺度下的熔点一致; 阳离子的比例对混合硝酸盐的相变温度有很大的影响, 且纳米线结构也会改变硝酸盐的相变温度. 硝酸盐的体热膨胀系数随着介孔尺度的增大而减小, 随着NaNO₃含量的增加而增大, 随着介孔结构的改变而改变. 离子之间的相互作用的增强会使导热率增大, 但对定压比热容没有太大影响.

关键词:

Abstract

Molecular dynamics method is used to simulate the influence of the mesopore size and structure on the heat transport characteristics of the mixed nitrate. The Material Studio software is used to establish the mixed nitrate models of different scales and two structures, and the NaNO₃-KNO₃ models of different proportions that reach the eutectic state. By calculating the models and sorting out the calculation results, the phase transition of mixed nitrates on a nanometer scale is calculated and the micro-mechanism of heat transport characteristics is analyzed. The results show that the phase transition temperature of the solar salt first increases and then decreases with the increase of the nanopore size, and finally is consistent with the melting point on a macro scale. The proportion of cations has a great influence on the phase transition temperature of mixed nitrate, and the nanowire structures also change the phase transition temperature of nitrate. The bulk thermal expansion coefficient of nitrate decreases with the increase of mesoporous size, increases with the increase of NaNO₃ content, and changes with the mesoporous structure. The enhancement of the interaction between ions will increase the thermal conductivity, but it will not have much effect on the specific heat capacity at a constant pressure.

Keywords:

作者及机构信息

青岛大学机电工程学院, 青岛　266071

通信作者: 杨启容, luyingyi125@163.com

基金项目: 国家自然科学基金(批准号: 51701102)资助的课题

Authors and contacts

College of Mechanical and Electrical Engineering, Qingdao University, Qingdao 266071, China

Corresponding author: Yang Qi-Rong, luyingyi125@163.com

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 51701102)

文章全文 : translate this paragraph

参考文献

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施引文献

图 1 NaNO₃和KNO₃的单晶胞

Fig. 1. NaNO₃ and KNO₃ single crystal cells.

下载: 全尺寸图片幻灯片

图 2 混合硝酸盐模型　(a) w (NaNO₃)∶w (KNO₃) = 4∶6混合硝酸盐; (b) w (NaNO₃) ∶w (KNO₃) = 5∶5混合硝酸盐; (c) w (NaNO₃) ∶w (KNO₃) = 9∶1混合硝酸盐; (d) w (NaNO₃)∶w (KNO₃) = 6∶4太阳盐; (e) w(NaNO₃)∶w (KNO₃) = 6∶4异结构太阳盐

Fig. 2. Mixed nitrate model: (a) w (NaNO₃)∶w (KNO₃) = 4∶6 mixed nitrate; (b) w (NaNO₃)∶w (KNO₃) = 5∶5 mixed nitrate; (c) w (NaNO₃)∶w (KNO₃) = 9∶1 mixed nitrate; (d) w (NaNO₃)∶w (KNO₃) = 6∶4 solar salt; (e) w (NaNO₃)∶w (KNO₃) = 6∶4 heterogeneous solar salts.

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图 3 不同温度下离子之间的径向分布函数　(a) w(K⁺)-w(Na⁺); (b) w(K⁺)-w(N^–); (c) w(Na⁺)-w(N^–)

Fig. 3. Radial distribution function of ions at different temperatures: (a) w(K⁺)-w(Na⁺); (b) w(K⁺)-w(N^–); (c) w(Na⁺)-w(N^–).

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图 4 不同尺度下离子之间的径向分布函数和相互作用能　(a) n(K⁺)-n(Na⁺); (b) n(K⁺)-n(N^–); (c) n(Na⁺)-n(N^–); (d)相互作用能

Fig. 4. Radial distribution function and interaction energy of ions at different scales: (a) n(K⁺)-n(Na⁺); (b) n(K⁺)-n(N^–); (c) n(Na⁺)-n(N^–); (d) interaction energy.

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图 5 不同比例下离子之间的径向分布函数和相互作用能(w(NaNO₃):w(KNO₃))　(a) w(K⁺)-w(Na⁺); (b) w(K⁺)-w(N^–); (c) w(Na⁺)-w(N^–); (d)相互作用能

Fig. 5. Radial distribution function and interaction energy of ions at different proportions (w(NaNO₃):w(KNO₃)): (a) w(K⁺)-w(Na⁺); (b) w(K⁺)-w(N^–); (c) w(Na⁺)-w(N^–); (d) interaction energy.

下载: 全尺寸图片幻灯片

图 6 两种结构下离子之间的径向分布函数和相互作用能　(a) n(K⁺)-n(Na⁺); (b) n(K⁺)-n(N^–); (c) n(Na⁺)-n(N^–); (d)相互作用能

Fig. 6. Radial distribution function and interaction energy of ions at two structures: (a) n(K⁺)-n(Na⁺); (b) n(K⁺)-n(N^–); (c) n(Na⁺)-n(N^–); (d) interaction energy.

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图 7 离子数为2760的太阳盐的均方位移和自扩散系数　(a)均方位移; (b)自扩散系数

Fig. 7. Mean square displacement and self diffusion coefficient of solar salt with ion number of 2760: (a) Mean square displacement; (b) self diffusion coefficient.

下载: 全尺寸图片幻灯片

图 8 不同尺度下太阳盐的体热膨胀系数和体积　(a)体热膨胀系数; (b)体积

Fig. 8. Thermal expansion coefficient and volume of solar salts at different scales: (a) Thermal expansion coefficient; (b) volume.

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图 9 不同比例下太阳盐的体热膨胀系数和体积(w(Na⁺)∶w(K⁺))　(a)体热膨胀系数; (b)体积

Fig. 9. Thermal expansion coefficient and volume of solar salts at different proportions (w(Na⁺)∶w(K⁺)): (a) Thermal expansion coefficient; (b) volume.

下载: 全尺寸图片幻灯片

图 10 两种结构下太阳盐的体热膨胀系数和体积　(a)体热膨胀系数; (b)体积

Fig. 10. Thermal expansion coefficient and volume of solar salts at two structures: (a) Thermal expansion coefficient; (b) volume.

下载: 全尺寸图片幻灯片

图 11 不同尺度下太阳盐导热率

Fig. 11. Thermal conductivity of solar salts at different scales.

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图 12 不同比例下混合硝酸盐导热率

Fig. 12. Thermal conductivity of mixed nitrates at different ratios.

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图 13 不同尺度下太阳盐定压比热容

Fig. 13. Fixed-pressure specific heat capacity of solar salts at different scales.

下载: 全尺寸图片幻灯片

图 14 不同比例(w(Na⁺)∶w(K⁺))下混合硝酸盐定压比热容

Fig. 14. Fixed-pressure specific heat capacity of mixed nitrate at different ratios (w(Na⁺)∶w(K⁺)).

下载: 全尺寸图片幻灯片

表 1 太阳盐($w({\rm NaNO_3}): w({\rm KNO_3}) = 6:4$)中NaNO₃和KNO₃的离子数

Table 1. Ion numbers of NaNO₃ and KNO₃ in solar salts ($w({\rm NaNO_3}): w({\rm KNO_3}) = 6: 4$)

离子数种类 Model size/nm
Na⁺ K⁺ N^– O^2–

460 60 32 92 276 5
920 120 64 184 552 5
1380 180 96 276 828 8
1840 240 128 368 1104 8
2300 300 160 460 1380 10
2760 360 192 552 1656 10

下载: 导出CSV

表 2 混合硝酸盐中NaNO₃和KNO₃的离子数(总离子数为460)

Table 2. Ion numbers of NaNO₃ and KNO₃ in mixed nitrate (total number of ions is 460).

$w({\rm NaNO_3}): w({\rm KNO_3})$ 种类 Model
size/nm
Na⁺ K⁺ N^– O^2–

4∶6 41 51 92 276 5
5∶5 49 43 92 276 5
6∶4 60 32 92 276 5
9∶1 84 8 92 276 5

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表 3 不同尺度下太阳盐的相变温度

Table 3. Phase transition temperature of solar salts at different scales.

离子数
460 920 1380 1840 2300 2760 5520

温度/K 493 493 503 518 508 492 493

下载: 导出CSV

表 4 不同比例的混合硝酸盐的相变温度

Table 4. Phase transition temperature of mixed nitrates at different proportions

w(NaNO₃)∶w(KNO₃)
4∶6 5∶5 6∶4 9∶1

温度/K 493 488 493 548

下载: 导出CSV

表 5 纳米线结构太阳盐的相变温度

Table 5. Phase transition temperature of nanostructured solar salts.

离子数
460 920

温度/K 528 548

下载: 导出CSV

表 6 两种结构下太阳盐导热率

Table 6. Thermal conductivity of solar salts at two structures.

离子数
460-
纳米孔 920-
纳米孔 460-
纳米线 920-
纳米线

导热率/(W·m^–1·K^–1) 0.46 0.63 0.99 1.98

下载: 导出CSV

map

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[6]	Deng Y, Qian T T, Guan W M 2017 J. Mater. Sci. Technol. 33 198 Google Scholar
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[11]	冯妍卉, 冯黛丽, 张欣欣 2019 介孔复合材料的相变及热输运特性 (北京: 科学出版社) 第5−138页 Feng Y H, Feng D L, Zhang X X 2019 Phase Transition and Thermal Transport Properties of Mesoporous Composite (Beijing: Science Press) pp5−138 (in Chinese)
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[13]	Bore M T, Pham H N, Switzer E E 2005 J. Phys. Chem. B 109 2873 Google Scholar
[14]	Zhang J R, Feng Y H, Yuan H B 2015 Comput. Mater. Sci. 109 300 Google Scholar
[15]	Wang L P, Sui J, Zhai M 2015 J. Phys. Chem. C 119 18697 Google Scholar
[16]	赵亚溥 2012 表面与界面物理力学 (北京: 科学出版社) 第212−220页 Zhao Y P 2012 Physical Mechanics of Surfaces and Interfaces (Beijing: Science Press) pp212−220 (in Chinese)
[17]	李亚琼, 梁凯彦, 王静静, 黄秀兵 2020 工程科学学报 42 1229 Google Scholar Li Y Q, Liang K Y, Wang J J, Huang X B 2020 J. Eng. Sci. 42 1229 Google Scholar
[18]	Min X, Fang M H, Huang Z H 2015 Sci. Rep. 5 12964 Google Scholar
[19]	Gao J K, Tao W W, Chen D 2018 Nanomaterials 8 385 Google Scholar
[20]	Sirota E B 2007 Macromolecules 40 1043 Google Scholar
[21]	冯黛丽, 冯妍卉, 张欣欣 2013 62 083602 Google Scholar Feng D L, Feng Y H, Zhang X X 2013 Acta Phys. Sin. 62 083602 Google Scholar
[22]	Asegun H, Chen G 2008 Phys. Rev. Lett. 101 235502 Google Scholar
[23]	黄丛亮, 冯黛丽, 张欣欣, 李静, 王戈, 侴爱辉 2013 62 026501 Google Scholar Huang C L, Feng Y H, Zhang X X, Li J, Wang G, Chou A H 2013 Acta Phys. Sin. 62 026501 Google Scholar
[24]	Ni H O, Wu J, Sun Z 2019 Chem. Eng. J. 377 120029 Google Scholar
[25]	Elena N, Anabel P, Tomos H 2017 Energy Stor. Sci. Tech. 6 688
[26]	吴玉庭, 王涛, 马重芳 2012 太阳能学报 33 148 Google Scholar Wu Y T, Wang T, Ma C F 2012 J. Sol. Energy 33 148 Google Scholar
[27]	官云许, 杨启容, 何卓亚, 王力伟 2021 功能材料 52 2153 Google Scholar Guan Y X, Yang Q R, He Z Y, Wang L W 2021 Funct. Mater. 52 2153 Google Scholar
[28]	李成祥, 孟庆元, 杨立军 2008 哈尔滨工业大学学报 40 705 Google Scholar Li C X, Meng Q Y, Yang L J 2008 Journal of Harbin Institute of Technology 40 705 Google Scholar
[29]	Pan G, Ding J, Wang W L 2016 Int. J. Heat Mass Transf. 103 417 Google Scholar
[30]	宫薛菲, 杨启容, 姚尔人, 刘亭 2020 功能材料 51 1214 Google Scholar Gong X F, Yang Q R, Yao E R, L T 2020 Funct. Mater. 51 1214 Google Scholar
[31]	Jayaraman S, Thompson A P, von Lilienfeld O Anatole 2010 Ind. Eng. Chem. Res. 49 559 Google Scholar
[32]	Anagnostopoulos A, Alexiadis A, Ding Y 2019 Sol. Energy Mater. Sol. Cells 200 109897 Google Scholar
[33]	倪海鸥, 孙泽, 路贵民 2017 储能科学与技术 6 669 Google Scholar Ni H O, Sun Z, Lu G M 2017 Energy Stor. Mater. 6 669 Google Scholar
[34]	车德勇, 沈辉, 蒋文强 2015 无机盐工业 47 30 Che D Y, Shen H, Jiang W Q 2015 Inorganic salt industry 47 30
[35]	Couchman P R, Jesser W A 1977 Nature 269 481 Google Scholar
[36]	David T B, Lereah Y, Deutscher G 1995 Philos. Mag. A 71 1135 Google Scholar
[37]	Reiss H, Wilson I B 1948 J. Colloid Sci. 3 551 Google Scholar
[38]	王海龙, 王秀喜, 梁海弋 2005 金属学报 41 568 Google Scholar Wang H L, Wang X X, Liang H Y 2005 J. Metal Sci. 41 568 Google Scholar
[39]	姜小宝 2013 博士学位论文 (长春: 吉林大学) Jiang X B 2013 Ph. D. Dissertation (Changchun: Jilin University) (in Chinese)
[40]	Sememchenko V K 1961 Surface Phenomena in Metals and Alloys (Oxford Pergamon) pp2−81
[41]	温元凯, 李振民 1978 科学通报 23 225 Google Scholar Wen Y K 1978 Chin. Sci. Bull. 23 225 Google Scholar
[42]	Lonappan M 1955 Proceedings of the Indian Academy of Sciences-Section A 41 239 Google Scholar
[43]	张景胤 2017 硕士学位论文 (北京: 华北电力大学) Zhang J Y 2017 M. S. Thesis (Beijing: North China Electric Power University) (in Chinese)
[44]	Kenisarin M 2010 Renew. Sust. Energ. Rev. 14 955 Google Scholar
[45]	李杨 2018 硕士学位论文 (郑州: 郑州大学) Li Y 2018 M. S. Thesis (Zhengzhou: Zhengzhou University) (in Chinese)
[46]	王长宝 2013 硕士学位论文 (北京: 北京工业大学) Wang C B 2013 M. S. Thesis (Beijing: Beijing University of Technology) (in Chinese)

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介孔尺度及结构对混合硝酸盐热输运特性的影响