基于分子动力学的熔盐热物性研究进展

doi:10.19799/j.cnki.2095-4239.2023.0708

摘要/Abstract

摘要：

熔盐作为高温传热蓄热介质，在太阳能光热发电、火电厂灵活性改造等场景中广泛应用。本文首先对熔盐分子动力学的势函数进行归纳分析，发现针对硝酸盐更适合使用带有库仑力的Buckingham势函数，碳酸盐和氯化盐采用BMH势函数计算可以减小模拟误差。其次对熔盐热物性进行分析，发现加入 $C a 2 +$ 可以降低太阳盐的熔点但会增加其黏度，硝酸盐中随 $N O 2 -$ 浓度的增加比热容降低； $L i +$ 离子浓度的增加会提高氯化盐的比热容和热导率，但会导致模拟误差增大， $K +$ 离子浓度增加会导致比热容误差减小，但其余热物性计算误差增大；碳酸盐模拟误差相对较小，与实验数据吻合较好。 $K +$ 、 $L i +$ 等对模拟结果产生的误差较大，离子增多后离子间势能的增加导致部分粒子丢失，引入边界条件后边界效应的影响会使误差增大。通过增加整体分子数量、校正位能截断距离、增加模拟时间步长等方法来减小误差。目前对同种阳离子、不同阴离子的熔盐分子动力学研究比较欠缺，探究纳米流体对熔盐分子动力学的影响、降低分子动力学模拟误差、开展基于分子动力学的熔盐腐蚀特性研究可以作为下一步熔盐分子动力学的研究方向。

关键词: 熔盐, 分子动力学, 势函数, 热物性

Abstract:

As a high-temperature heat transfer and storage medium, molten salt is widely used for solar thermal power generation and the flexible transformation of thermal power plants. First, the potential functions of the molecular dynamics of molten salt were summarized and analyzed. This indicated that to reduce simulation errors, the Buckingham potential with coulomb force is more suitable for nitrate and the BMH potential is more suitable for carbonate and chloride salt. Second, an analysis of the thermal properties of molten salt indicated that the addition of Ca²⁺ to solar salt decreased its melting point and increased its viscosity, and the specific heat capacity of nitrate decreased with increasing NO^2- concentration. Increased Li⁺ concentrations increased the specific heat capacity and thermal conductivity of chloride salt but also increased the simulation error; however, with increased K⁺, the specific heat capacity error decreased and the error when calculating residual heat properties increased. The carbonate simulation error was relatively small, which is consistent with experimental results. The simulation errors were large with the addition of K⁺ or Li⁺, and the increased potential energy between ions led to the loss of some particles. It was found that the influence of the boundary effect after the introduction of a boundary condition increased the error; however, the error was reduced by increasing the number of molecules, the potential energy truncation distance correction, and the simulation time step. Currently, studies on the molecular dynamics of molten salt with the same cation and different anions are rare. Exploring the influence of nanofluids on molten salt molecular dynamics, reducing the simulation error of molecular dynamics, and conducting research on the corrosion characteristics of molten salt based on molecular dynamics is the next research direction of molten salt molecular dynamics.

Key words: molten salt, molecular dynamics, potential function, thermophysical property

中图分类号:

TK 512

付殿威, 张灿灿, 娜荷芽, 王国强, 吴玉庭, 鹿院卫. 基于分子动力学的熔盐热物性研究进展[J]. 储能科学与技术, 2023, 12(12): 3873-3882.

Dianwei FU, Cancan ZHANG, Heya NA, Guoqiang WANG, Yuting WU, Yuanwei LU. Review of the molecular dynamics of molten salt thermal physical properties[J]. Energy Storage Science and Technology, 2023, 12(12): 3873-3882.

图/表 10

图1

图2

表1

熔盐分子动力学模拟势函数"

氯化物、硝酸根和碳酸根熔盐的模拟势函数
序号	势函数名称	应用类型	公式
1	Born-Mayer-Huggins-Tosi-Fumi^[24] (BMHFT)	$N a C l$	$ϕ i j r = Z i Z j e 2 r + A i j e x p B σ i + σ j - r - C i j r 6 - D i j r 8$	(1)
1	Born-Mayer-Huggins-Tosi-Fumi^[24] (BMHFT)	$N a C l$	$A i j = A i A j 12, C i j = C i C j 12, 2 ρ i j = 1 ρ i + 1 ρ j$	(2)
2	Born-Mayer-Huggins-Tosi-Fumi^[25](BMHFT)	$N a C l$	$Φ = Z i Z j e 2 4 π ε ε 0 r + B i j e x p - r - σ i j β i j - C i j r 6 - D i j r 8$	(3)
3	Born-Mayer-Huggins^[26](BMH)	$N a C l$ $- K C l$	$E i j = A i j e σ i j - r i j ρ - C i j r i j 6 - D i j r i j 8$	(4)
4	Born–Mayer–Huggins^[27-28](BMH)	$N a C l$ $- L i C l$ $- K C l$ $L i C l$ $- K C l$ $N a C l$ $- K C l$ $N a 2 C O 3$ $- K 2 C O 3$	$U i j = q i q j r i j + A i j e x p σ i j - r i j ρ - C i j r i j 6 - D i j r i j 8$	(5)
5	Born-Mayer^[29]	$N a 2 C O 3$ $- K 2 C O 3$ $L i 2 C O 3$	$u r i j = z i z j e 2 r i j + b 1 + z i n i + z j n j e x p α σ i + σ j - r i j$	(6)
6	Busing^[30]	$Z n C l 2$ $Z n C l 2$ $- K C l$	$φ i j = - Z i Z j r i j + f ρ i + ρ j e x p R i + R j - r i j ρ i + ρ j$	(7)
7	Buckingham^[31]+Coulomb^[32]	$N a N O 3$	$U B u c k i n g h a m = ∑ i ∑ i ≠ j A i j e - r i j ρ i j - C i j r i j 6, r i j < r c$	(8)
7	Buckingham^[31]+Coulomb^[32]	$N a N O 3$	$U C o u l o m b = ∑ i ∑ i ≠ j q i q j ε r i j, r i j < r c$	(9)
8	Buckingham^[33]	$N a N O 3$ $- K N O 3$ $K 2 C O 3$ $- L i N O 3$ $N a N O 3$ $- K N O 3$ $- N a N O 2$	$E = A i j e - r i j ρ i j - C i j r i j 6 + q i q j 4 π ε 0 r i j$	(10)
9	Lennard-Jones^[34](LJ)	$N a N O 3$ $- K N O 3$ $N a C l$	$E r = q i q j r + 4 ε σ r 12 - σ r 6$	(11)
9	Lennard-Jones^[34](LJ)	$N a N O 3$ $- K N O 3$ $N a C l$	$σ i j = σ i + σ j 2, ε i j = ε i ε j$	(12)

表1

表2

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序号	名称	公式
1	径向分布函数RDF	$g α β r = 1 4 π ρ β r 2 d N α β r d r$	(13)
2	配位数N(r)	$N α β r = 4 π ρ β ∫ 0 r m i n g α β r r 2 d r$	(14)
3	均方位移MSD	$M u t = r t - r 0 2$	(15)
4	自扩散系数D^[35]	$D u = 16 d M u t d t$	(16)
5	角分布函数ADF	$θ i j k = c o s - 1 r i j 2 + r i k 2 - r j k 2 2 r i j r i k$	(17)
6	密度^[36]	$ρ = N M V N A$	(18)
7	比热容	$C p = Q / Δ T$	(19)
8	剪切黏度^{[24, 37]}	$η = 1 k B T V ∫ 0 ∞ P x y 0 P x y t d t$	(20)
8	剪切黏度^{[24, 37]}	$P x y t = ∑ i = 1 N m i v x i v y i + 12 ∑ j ≠ i x i j f y r i j$	(21)
9	热导率	$j z = - λ T ∂ T ∂ z$	(22)
9	热导率	$λ T = - ∑ t r a n s f e r m 2 v h o t 2 - v c o l d 2 2 t L x L y ∂ T / ∂ z$	(23)
10	离子电导率^[38]	$λ z = 1 3 V k B T ∫ 0 ∞ J z 0 J z t d t$	(24)
11	键能^[39]	$E = K b (r - r 0) 2 + K a (θ - θ 0) 2 + K u b (r - r u b) 2$	(25)

熔点	介孔尺寸
熔点	3 nm	4 nm	6 nm
实验结果/K	485.45	488.71	499.16
模拟结果/K	492	493	503

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