1 s2.0 S2352152X2300169X Main

Journal of Energy Storage 61 (2023) 106772
Contents lists available at ScienceDirect
Journal of Energy Storage

journal homepage: www.elsevier.com/locate/est
Review article
Progress of research on phase change energy storage materials in their

thermal conductivity
Shenhui Tan, Xuelai Zhang *
Institute of Cool Thermal Storage Technology, Shanghai Maritime University, Shanghai 201306, China
A R T I C L E I N F O A B S T R A C T
Keywords: In recent years, phase change materials (PCM) have become increasingly popular for energy applications due to
Phase change materials their unique properties. However, the low thermal conductivity of PCM during phase change can seriously hinder
Thermal conductivity its wide application, so it is crucial to improve the thermal conductivity of PCM. In this paper, the thermal
Thermal conductivity mechanism
conductivity mechanism of PCM (basic thermal conductivity, phonon thermal conductivity and channel thermal
Thermal conductivity prediction models
conductivity) and thermal conductivity prediction models (nano-type and foam-metal type) are systematically
Nanomaterials
Metal foams discussed from a microscopic perspective, providing a theoretical basis and a validation model for the study of
External fields thermal conductivity of PCM. In addition, we review three specific approaches to improve PCM from a
macroscopic perspective: addition of nanoparticles, embedded foam structures, and addition of external fields.
Finally, it is concluded that the specific approaches to improve the thermal conductivity of PCM all proceed to
enhance the different thermal conductivity mechanisms of PCM, and future research directions to improve the
thermal conductivity of PCM are proposed in response to this conclusion.
Phase change materials are substances that change the state of

matter at constant temperature and can provide latent heat, which can
1. Introduction be divided into organic phase change materials, inorganic phase change
materials and composite phase change materials, as shown in Fig. 1.
At the 75th session of the United Nations General Assembly, the Organic PCM has the advantages of high latent heat, wide phase change
Chinese government aims to reach peak carbon emissions by 2030 and temperature, non-toxic, non-corrosive and cheap, but also has the dis
strives to achieve carbon neutrality by 2060. The conversion and opti advantages of low thermal conductivity and easy leakage during phase
mization of the energy mix under this goal have become an indispens change [10]. Organic PCM is mainly divided into paraffin and non-
able part [1]. At present, new energy sources mainly include solar paraffin waxes, while non-paraffin waxes are generally fatty acids, al
energy, wind energy, tidal energy, etc. However, these energy sources cohols, esters, etc. [11–14] Compared with organic PCM, inorganic PCM
are affected by environmental and time factors with intermittency and has greater thermal conductivity and heat storage, but severe subcooling
randomness, so energy storage becomes especially important and be and phase separation can occur during the phase change process [15]. It
comes a key technology to solve the energy crisis [2]. The thermal en mainly has crystalline hydrated salts, molten salts, metal alloys, etc.
ergy storage methods can be classified as sensible heat storage (SHS) [3], [16–18] Composite PCMs are generally obtained by compounding two
latent heat storage (LHS) [4] and thermochemical storage [5], where PCMs, adding nanoparticles, and embedding foam structures, as detailed
PCM absorbs and releases heat as latent heat during the phase change. in Part 3 of this paper.
Phase change energy storage materials can solve the uneven distribution
of energy in space and time on the one hand, on the other hand, phase
change energy storage materials have the advantages of temperature 1.1. Research on the thermal conductivity of PCM in recent years
stability, high energy storage density and large energy storage capacity,
which makes phase change energy storage materials can be applied to Thermal conductivity is a key parameter for phase change energy
various fields. For example, in the aerospace sector [6], in the building storage systems to measure how fast or slow the energy is transferred.
energy-saving field [7], in industrial waste heat utilization [8], and in Many researchers in China and abroad have done a lot of work on
the apparel industry field [9]. improving the thermal conductivity of phase change materials. Laghari
* Corresponding author.
E-mail address: xlzhang@shmtu.edu.cn (X. Zhang).
https://doi.org/10.1016/j.est.2023.106772
Received 27 October 2022; Received in revised form 15 December 2022; Accepted 27 January 2023
Available online 8 February 2023
2352-152X/© 2023 Elsevier Ltd. All rights reserved.
S. Tan and X. Zhang Journal of Energy Storage 61 (2023) 106772
Nomenclature Subscripts
A unit cell subsection
a1 geometrical parameter controlling cross-sectional shape of B unit cell subsection
ligament, [− ] C unit cell subsection
k thermal conductivity, [W/(m.K)] D unit cell subsection
H height of nanorod, [nm] eff effective
R thermal resistance on a flux basis, [m2KW− 1] f basefluid
T temperature, [K] s solid-phase
L node-to-node length, [m] p particle (rod)
Cp specific heat, [J/kg.K]
a aspect ratio of Nanoparticle,[− ] Abbreviations
e dimensionless cubic node length,[− ] PCM Phase change materials
g dimensionless foam ligament radius,[− ] CBM Carbon based nanomaterials
t thickness of the interfacial layer, [nm] CBNP Carbon black nanoparticles
d diameter,[m] CNT Carbon nanotubes
r radius of nanorod, [nm] SWCNT Single-walled carbon nanotubes
x,z x-axis, z-axis,[− ] MWCNT Multi-walled carbon nanotubes
GO Graphene oxide
Greek letters HTC Hydrothermal carbon
ϕ volume fraction of nanoparticles,[%] PEG Polyethylene glycol
ρ density, [kg/m3] EG Expanded graphite
δ The metal foam porosity,[− ] GF Graphite foam
φ solidity of ligament,[− ] rGOS Graphene sponge
θ imensionless parameter,[− ] MP-LA/PAN Methyl palmitate-lauric acid/acrylonitrile composite
phase change fibres
adsorbed a binary eutectic mixture of octanoic acid-myristic acid (OA-

MA) onto graphite with porous structure, which significantly improved
3DUD⒑QZD[ the thermal conductivity of OA-MA. Bao et al. [21] used scale graphite
to reduce the subcooling of CaCl2⋅6H2O and also used a highly absorbent
polymer as a thickener to improve the resistance to dissociation of liquid
2UJDQLF3KDVH CaCl2⋅6H2O, and scale graphite also improved the thermal conductivity
)DWW\DFLGV of PCM. Hirschey et al. [22] used the extended one-pot synthesis process
&KDQJH0DWHULDOV
to prepare salt hydrate-graphite composite materials, and used three
kinds of graphite, including expanded graphite (EG), ground expanded
$OFRKROV graphite (MG) and graphene nanosheet (GnP), to improve the thermal
conductivity of sodium sulfate decahydrate (SSD).
In recent years, since PCM can provide heat absorption effect to
3KDVHFKDQJH
,QRUJDQLFVDOWV reduce the operating temperature of the battery, the PCM-based thermal
PDWHULDOV
management system for cooling battery has gradually become a hot

research topic [23]. However, the vulnerability to leakage, low thermal
,QRUJDQLFSKDVH conductivity and rigidity of PCM limit its application in battery thermal
0ROWHQ6DOW
FKDQJHPDWHULDOV management. To address its low thermal conductivity aspect, Xiangwei
Lin et al. [24] used styrene-ethylene-propylene-styrene as a support
material to prevent PCM leakage, while expanded graphite was used to
0HWDOVDQGDOOR\V improve its thermal conductivity. And Chuyuan Ma et al. [25] went to
enhance the thermal conductivity of PCM by adding two types of ma
terials, expanded graphite and copper nanoparticles. Also, Yanan Wang
2UJDQLF,QRUJDQLF et al. [26] found that increasing the thickness of PCM cells can improve
the thermal management performance in a passive low-cost battery
thermal management system consisting of a pouch Li-ion battery and a
&RPSRVLWHSKDVH phase change material cell. However, exceeding the limit of 6 mm af
2UJDQLF2UJDQLF
FKDQJHPDWHULDOV fects the thermal management performance.
,QRUJDQLF
1.2. Contribution of this study
,QRUJDQLF
Thermal conductivity is one of the most important material proper
Fig. 1. Schematic diagram of the classification of phase change materials.
ties that affect the performance index of PCM in energy storage systems.
In short, the thermal conductivity of PCM directly affects the heat
et al. [19] improved the thermal conductivity with organic phase change
transfer rate during the storage and release of thermal energy, so the
material paraffin wax (PW) as well as its latent heat value by adding
efficiency of the energy storage system will be influenced by its thermal
titanium dioxide - graphene (TiO2:Gr) binary composites with sodium
conductivity. Based on the importance of phase change energy storage
dodecyl benzene sulfonate (SDBS) as surfactant. Zhou Sunxi et al. [20]
materials in the energy field and the key role of their thermal
2
conductivity parameters. This paper reviews the research progress of that natural convection of erythritol material during melting had a
PCM in its thermal conductivity from both microscopic and macroscopic significant effect on the device by studying the phase transition of
perspectives. The contributions of this study are as follows: erythritol in a horizontal shell multi-pin tube device, and that heat
conduction dominated during solidification without subcooling. How
• This paper provides a comprehensive summary and classification of ever, Shiquan He et al. [29] also studied the heat transfer characteristics
the existing thermal conductivity mechanisms and thermal conduc of organic PCM erythritol phase transition, but clearly subdivided the
tivity prediction models for PCM, and provides a theoretical basis for melting process into three stages, namely, channel formation stage (heat
the subsequent development of its novel optimization approach. conduction), melting stage (dominated by convection heat transfer) and
• According to the existing studies on the thermal conductivity final stage (storage by sensible heat). There are two stages of latent heat
mechanism of PCM, there is a deficiency. Most of the studies are storage: channel formation and melting. This means that the convective
proposed for solid-liquid PCM, and there are fewer studies on the heat exchange mechanism gradually increases with the time of the PCM
thermal conductivity mechanisms of both solid-gas and liquid-gas melting process, while the solidification process is the opposite [30].
types. This paper provides an idea for the study of solid-gas and At the same time, in order to ensure the efficiency of phase change
liquid-gas thermal conductivity mechanisms in response to the above material storage and discharge, it is necessary to reduce the melting/
limitations, as detailed in the outlook (1) in Section 4 of this paper. solidification time of PCM from heat conduction and thermal convection
• By analyzing the existing PCM thermal conductivity prediction mechanism. In the melting process of phase change materials, convec
models, it is found that they can be broadly classified into nanotypes tive heat transfer is the main heat transfer mechanism. Increasing
and foam-metal types. However, the accuracy of the models needs to external factors such as external temperature, external air flow rate and
be improved, and fewer types of thermal conductivity prediction panel tilt angle can influence the promotion of natural convection to
models other than nanotypes and foam-metal types have been reduce melting time and provide energy release efficiency [31]. Wei Cui
developed, leading to a limited range of applications. This paper et al. [32] also enhanced convective heat transfer by using ultrasonic
provides specific paths to solve the above problems in the outlook(2) waves on phase change materials to produce a cavitation effect thereby
(3)(4) in Section 4. increasing the flow rate of the liquid during the melting process of the
• The existing specific ways to improve the thermal conductivity of phase change material. Xuan Zhang et al. [33] used gallium as the
PCM are reviewed and can be divided into three types: addition of premise of filling phase change material to increase the heat transfer by
nanoparticles, embedded foam structures, and addition of external adding the number of fins found that there is a competing mechanism
fields. However, most of the existing studies use a single enhance between thermal conductivity and convective heat transfer during the
ment modality, and fewer studies use more than two modalities to melting and solidification of the phase change material. As the number
act together on PCM. Therefore, we can combine various methods to of fins increases, the thermal conductivity of the specific surface area
improve the thermal conductivity of PCM, and explore its action law between the PCM and the fins is enhanced, while the reduced fin spacing
to achieve further optimization. inhibits natural convection, which also results in a much shorter melting
time and a delayed solidification process for the PCM.
1.3. Outline of this article However, the heat transfer mechanism in the melting process of PCM
embedded in metal foam is not dominated by convective heat transfer,
The rest of this paper is organized as follows. In Section 2, three PCM but by heat conduction. This is because from the micro-scale heat
thermal conductivity mechanisms and two major thermal conductivity transfer, it is concluded that the presence of foam metal skeleton acts as
prediction models are analyzed and summarized in detail. In Section 3, the heat transfer channel of phase change materials, so heat conduction
three specific methods to improve the thermal conductivity of PCM are is the main heat transfer mechanism in the melting process of PCM [34].
reviewed. Finally, in Section 4, its internal mechanism and specific At the same time, the attenuation of convective heat transfer in liquid
methods for improvement are summarized, along with an outlook on phase PCM is also an important reason due to the limitation of foam
them. metal framework. Zilong Wang et al. [35] also used paraffin wax as the
phase change material and added copper foam to it to prepare composite
2. Phase change material thermal conductivity mechanism and phase change materials with copper foam ratio increasing from 0 % to
thermal conductivity prediction model 2.13 %, respectively, and by studying the melting process of copper
foam composite phase change materials, it was found that as the CMF
2.1. Thermal conductivity mechanism of phase change materials ratio increased from 0.43 % to 2.13 %, the natural convection ratio
decreased from 62.1 % to 7.7 % (results shown in Fig. 2), indicating that
2.1.1. Basic heat transfer mechanism convective heat transfer is the main heat transfer mechanism in the
The basic heat transfer mechanism of phase change materials is melting process of low copper foam ratio composite phase change ma
mainly heat conduction and convection heat transfer. When the physical terials and heat conduction is the main heat transfer mechanism in the
state of the phase change material is a solid, the heat transfer on the melting process of high copper foam ratio composite phase change
insulating solid is caused by the thermal vibration of the solid lattice, i. materials.
e., the phonon conduction mechanism as described in Section 2.1.2. In For the numerical simulation part of the heat conduction and
contrast, heat conduction on metals and other non-insulated conductors convective heat transfer mechanism of phase change materials, Mišo
is caused by thermal vibrations of the lattice and free electron move Jurčević et al. [36] developed for the first time a real-time numerical
ment, i.e. phonon and electron conduction [27]. When the phase change model capable of simulating higher scale solidification and melting in
material is in liquid state, the thermal conductivity of the phase change order to study the transient solidification of phase change materials
material is convective heat transfer. However, since we know that solid- dominated by convective heat transfer. Peiyi Li et al. [37] constructed a
liquid coexistence is inevitable in the phase change process of phase physical model of a slender rectangular cavity to numerically study the
change materials, it is very important to analyze which is dominant in paraffin melting process, and also used several dimensionless parame
the process of phase transition, heat conduction or convection heat ters such as Reynolds number Re and Rayleigh number Ra as quantita
transfer. tive indicators to describe and evaluate the heat transfer mechanism in
Usually, solid-liquid phase change materials store energy in a so the cavity, and found that the convective heat transfer efficiency of PCM
lidification process and release energy in a melting process. Domestic in the melting process can be achieved by increasing the Reynolds
and foreign studies for the analysis of the thermal conductivity mecha number Re and Rayleigh number Ra.
nism during melting and solidification. Firstly, R. Anish et al. [28] found
3
Fig. 2. Effect of the CMF proportion on the heat conduction and natural con
vection in the melting process of the composite PCMs [35].
2.1.2. Phonon heat transfer mechanism

Phonon conduction exists in the solid state of phase change mate
rials, whether insulated or non-insulated, and phonons are the driving
force responsible for transferring heat from one end to the other, so the Fig. 4. Schematic diagram of three phonon scattering modes [38].
study of phonon conduction mechanisms in micro-scale heat transfer is
of great significance in controlling the thermal conductivity of phase phonons. Generally, the higher the temperature, the more intense the
change materials. The phonon heat transfer process is shown in Fig. 3. collisions, the shorter the mean free path and the higher the thermal
The atoms acquire thermal energy and give it to neighboring atoms in conductivity. For example, after grafting functional groups on the phase
the form of vibrational waves, which then diffuse throughout the ma change material, the thermal resistance of the interface between the
terial and finally when transferred to the back of the material by con functional group and the phase change material decreases, thus the
duction or radiation to the outside world. phonon scattering decreases, the average free range of phonons in
Shaofei Wu et al. [38] reviewed the main influencing factors of creases, and the thermal conductivity of the phase change material
phonon transport including phonon velocity, specific heat capacity, and increases.
mean free range. Particular attention should be paid to the fact that in Fewer systematic studies analyze the thermal conductivity of phase
non-metallic phase change materials, phonon scattering is the main change materials from the microscopic perspective of phonon heat
cause of the thermal conductivity of the material, and phonon scattering conduction, but many researchers inevitably refer to phonon heat con
causes the energy to be transferred in the opposite direction of the duction mechanisms when studying thermal conductivity. For example,
original. Phonon scattering can be divided into three parts: phonon- Haoxiang Lyu et al. [39] improved the thermal conductivity of the
phonon scattering, phonon defect scattering and phonon interface composite by 245 % when the graphene nanosheets (GNS) were doped
scattering, as shown in Fig. 4. In general, the temperature dependence of at 3.0 wt%, due to a better phonon vibration match between GNS and
the thermal conductivity depends on the specific heat capacity and is sodium nitrate. C.Y. Zhao et al. [40] studied the thermal and phonon
proportional to the absolute temperature (T). The mean free path of transport characteristics through MD simulation, and revealed that the
phonons refers to the average distance traveled by collisions between weakening of phonon scattering in the nanolayer was the internal
Fig. 3. Spring vibration heat transfer system composed of crystal atoms and abstract phonons [38].
4
mechanism for improving the thermal conductivity of NPCM. two cases.
2.1.3. Channel heat transfer mechanism 2.2.1. Nanoparticle type

Organic phase change materials themselves carry functional groups, The earliest EPCM thermal conductivity prediction model is gener
and these can be understood as heat transfer channels, and different ally accepted in academia as the Maxwell model [46], but this model is
functional groups have channels with different heat propagation rates. only applicable to phase change materials where the nanoparticles are
For example, multi-walled carbon nanotubes (MWCNT) contain hy spherical. Later EVERY [47] changed the particle shape of the packing to
droxyl (–OH), carboxyl (–COOH) and amino (–NH2) groups, and the derive a theoretical model of thermal conductivity applicable to ellip
influence of functional groups on the phase transition behavior of soidal packing. Domestic and international thermal conductivity pre
composite PCM follows the following order: MWNT-COOH > MWNT- diction models based on Maxwell's equation for nanofluid particle
NH2 > MWNT-OH > MWNT [41]. shapes are shown in Table 1.
Not only the functional groups are part of the channel heat transfer In addition to developing various thermal conductivity prediction
mechanism, but also the interaction forces existing between the func models for nanoparticle shapes, researchers have continued to refine
tional groups are part of the channel heat transfer mechanism. Hiroki thermal conductivity prediction models considering the nanofluid mo
Matsubara et al. [42] analyzed the molecular heat transfer mechanism of tion, viscosity, temperature, and particle volume concentration. Koo
linear alcoholic liquids based on atomic heat path (AHP) analysis and et al. [54] combined the Maxwell thermal conductivity prediction model
showed that the hydroxyl group does not act as a heat carrier in the with the Brownian motion of nanofluids thereby developing a new
phase change material but provides the heat path for coulombic and thermal conductivity prediction model that takes into account particle
intermolecular interactions, as shown in Fig. 5. Biao Feng et al. [43] size, particle volume fraction and temperature dependence as well as the
analyzed the thermal conductivity of PE from the microscopic crystal nature of the base fluid and particle phases with the following equations:
structure of a solid-solid phase change material, pentaerythritol (PE), [ ( ) ] √̅̅̅̅̅̅̅̅̅
and verified by prediction and experiment that the main reason for the keff = kf
kp + 2kf − 2 kf − kp ϕ
( ) + 5 × 104 βϕρf Cpf
kT
f (T, ϕ) (1)
change in thermal conductivity during phase change is the breakage of kp + 2kf + kf − kp ϕ ρp dp
strong intermolecular hydrogen bonds (HBs) on the crystal structure due
to the increase in temperature and the formation of weak intermolecular where f(T, ϕ) was fitted by Vajjha et al. [55] using a curve to produce a
HBs. single correlation:
Therefore, one of the most common methods in improving the ( )T (
thermal conductivity of phase change materials is to increase the heat f(T, ϕ) = 2.8271 × 102 ϕ + 3.917 × 10− 3 + − 3.0669 × 10− 2 ϕ
T0 (2)
transfer channels, such as adding nanoparticles and embedding foam )
− 3.91123 × 10− 3
structures in PCM. For example, Zengkai Jiao et al. [44] increased the
thermal conductivity by using nickel particles as catalysts to grow car Also the thermal conductivity in nanofluidic composite phase change
bon nanotubes vertically onto a diamond film, treating the diamond materials is inevitably affected by the interfacial thermal resistance
skeleton as an “active” heat transfer and the carbon nanotubes as a [56], so several of the above predicted thermal conductivity models
“capillary” secondary heat transfer, and adding thermal conductivity have some errors with the actual experimental values. To address the
channels to the phase change material. effect of interfacial thermal resistance, researchers have developed the
Maxwell-Garnett type effective medium approach (EMA) [56], the
2.2. Prediction model for thermal conductivity of phase change materials improved Hamilton-Crosser model [57] and the Leong model [58],with
the equations shown in Table 2.
In recent years, the most common methods to improve the thermal Yanlin Song et al. [59] studied the prediction model of thermal
conductivity of phase change materials are the addition of nano conductivity of PCM composite of fatty acid and carbon materials based
materials (EPCM) to PCM and the filling of PCM into porous foams
[44,45]. The thermal conductivity prediction models of these two
methods are not quite the same, so the prediction models developed by Table 1
domestic and foreign researchers are presented below for each of these Thermal conductivity prediction model based on nanoparticle shape.
Model name Particle Model
shape
( )
Maxwell [46] Spherical kp + 2kf + 2ϕ kp − kf
keff = kf ( )
kp + 2kf − ϕ kp − kf
Bruggeman Spherical 1[ ] kf √̅̅̅
keff = (3ϕ − 1)kp + (2 − 3ϕ)kf + Δ
[48] 4 4
Δ = (3ϕ − 1)2(kp/kf)2 + (2 − 3ϕ)2 + 2(2 + 9ϕ −
9ϕ2)(kp/kf)
Bhattacharya Spherical keff = ϕkp + (1 − ϕ)kf
[49]
Timofeeva [50] Spherical keff = kf(1 + 3ϕ)
Xue [51] Nanotubes kp + kf
1 − ϕ + 2ϕ kp ln 2kf
kp − kf
keff = kf
kf kp + kf
1 − ϕ + 2ϕ ln
kp − kf 2kf
( )
Yamada-Ota Nanotubes Hkf 0.2 kf H
1+ ϕ + 1− ϕ ϕ0.2
[52] rkp kp r
keff = kf ( )
Hkf 0.2 kf
1+ ϕ − 1− ϕ
rkp kp
Yang [53] Nanorods (H + 2t)keff− x + (r + t)keff− z
keff =
H + r + 3t
Fig. 5. The model of Coulomb path for ethanol as an example. The charge
neutral group Q at the center has a Coulomb path with another Q inside the first keff-x: Effective thermal conductivity on the x-axis; keff-z: Effective thermal conduc
nonhydrogen-bond shell. The ± symbols of the constituent atoms of Q at the tivity in the z-axis; kp: Thermal conductivity of nanoparticles; kf: Thermal conduc
center show the sign of partial electric charge [42]. tivity of the base fluid.
5
Table 2 change materials, the models of machine learning methods are more
Thermal conductivity prediction model for solving interface thermal resistance. general and avoid some complicated computational processes. However,
Model Model Remarks one inevitable drawback of machine learning methods is that they
name require a sufficient amount of data to support them, and the quality of
Nan [3 + ϕ[2β (1 − L ) + β (1 − L ) ] ]
xx xz a2
the data needs to be guaranteed.
xx zx
keff = kf Lxx = +
[56] 3 − ϕ[2βxx (Lxx ) + βzz (Lz ) ] 2(a2 − 1)
a 2.2.2. Metal foam type
cos− 1 a
2(1 −
32
a2 )
/
From Section 2.1.3, we know that the thermal conductivity mecha
L∑z = (1 − 2Lxx) nism of filling the phase change material into the foam is to build heat
βxx = transfer channels, and the more channel networks, the faster the heat
transfer rate, the higher the thermal conductivity of this composite
kp,xx − kf
( ) phase change material. Therefore, when predicting the use of metal
kf + Lxx kp,xx − kf
foam to increase the thermal conductivity of phase change materials,
kp,xx = one should understand the microscopic geometric model of metal foam
as well as its ligament shape, orientation, vacuum, etc. The microscopic
dp
2Reff + dp
/ structure of metal foam is shown in Fig. 7.
kp,in− plane
For predicting the thermal conductivity of metal foam type com
ak = Rkkf
Yu [ kp/
⎤ posite phase change materials, researchers initially went on to derive a
ϕa kf two-dimensional thermal conductivity prediction model based on the
[57] keff = kf 1 + ⎦
3 2ak kp
a+
δ
×
kf
hexagonal structure of the foam metal matrix [62]. Later, Boomsma
Leong β = h/ et al. [63] developed a three-dimensional thermal conductivity predic
keff = r
[58] β1 = 1 + β 2 / tion model based on the structure of a foam matrix as a decahedron.
( ) (
kp − klayer ϕklayer 2β1 3 − β2 3 + 1
)
β2 = 1 + β However, the Boomsma-Poulikakos model ignores the metal foam lig
( ) ( ) (
β1 3 kp + 2klayer − kp − klayer ϕ β1 3 + β2 3 − 1
)+ klayer = 10kf ament orientation factor when calculating the effective thermal con
( ) 3( 3
(
kp + 2klayer β1 ϕβ2 klayer − kf + kf
) )
ductivity, so the calculated thermal conductivity has some errors. Dai
[64]. corrected and extended the Boomsma-Poulikakos model to take
( ) ( ) ( )
β1 3 kp + 2klayer − kp − klayer ϕ β1 3 + β2 3 − 1
into account the metal foam ligament orientation factor to make the
a:Nanoparticle Aspect Ratio; Reff: Effective interface thermal resistance; kp,xx:modi
effective thermal conductivity prediction more accurate, as shown in
fied in-plane thermal conductivity of Nanoparticle；kp,in-plane: In-plane thermal
conductivity of Nanoparticle; klayer: Nanosphere thermal conductivity; h: Nanosphere Table 3. Dongxu Wu et al. [61] developed a model for predicting the
thickness. effective thermal conductivity of open-cell foam composites based on
the orthopentagonal dodecahedral geometry model.
on the Sierpinski carpet model with fractal geometry, and found that the The effective thermal conductivity obtained using thermal conduc
QP prediction model and Maxwell-Eucken prediction model are more tivity prediction models inevitably has some error with the values from
accurate, as shown in Fig. 6. experimental studies, and there are two general methods to assess the
In recent years, not only special mathematical models have been accuracy of various foam-metal-based thermal conductivity prediction
developed to predict the thermal conductivity of different phase change models, namely the mean squared error (MSE) method [65] and the
materials for their characteristics [59], but also some machine learning relative deviation (RD) method [66]. MSE is defined as
methods have been used to do so. Jaliliantabar et al. [60] mainly
introduced three machine learning methods to predict the thermal
conductivity of nano-enhanced phase change materials, namely MARS
(multiple adaptive regression splines), CART (classification and regres
sion tree) and ANN (artificial neural network). Compared with past
mathematical models for predicting the thermal conductivity of phase
Fig. 7. Microstructure of open-cell foam: (a) the microstructure of the copper

Fig. 6. Comparison of fractal prediction model of CNTs with QP and Maxwell- open cell foam; (b) typical unit cell structure of the open cell foam; (c) tri-prism
Eucken prediction model [59]. solid ligaments; (d) hollow ligaments [61].
6
Table 3
Thermal conductivity prediction model based on foam metal substrate shape.
Model name Substrate shape Model Remarks
√̅̅̅
Boomsma Decahedron 2 4g
keff RA =
[63] =
2(RA + RB + RC + RD ) (2e2 + πg(1 − e) )ks + (4 − 2e2 − πg(1 − e) )kf
(e − 2g)2
RB =
(e − 2g)e2 ks + (2e − 4g − (e − 2g)e2 )kf
( √̅̅̅ )2
2 − 2e
RC = ( √̅̅̅ ) ( √̅̅̅ ( √̅̅̅ ) )
2πg 1 − 2e 2 ks + 2 2 − 2e − πg2 1 − 2e 2 kf
2
2e
RD = 2
e ks + (4 − e2 )kf
√̅̅̅
Dai [64] Decahedron LA + LB + Lc + LD LA + LB + Lc + LD = L 2/2
keff =
R′A + R′B + R′C + R′D RA′ = LRA
RB′ = LRB
RC′ = LRC
R′ D = LRD
Wu [61] Orthopentagonal (1 + a2 )[ ] { (1 + a2 )[
keff = k1 = 3.04 1
2φθ + (1 − 4φ)θ2 ks + 1 − 3.04 1
2φθ + (1 −
dodecahedron a21 a21
}
]
L 4φ)θ2 kf
(2L ) ( )H( ) ( )
1 2L2 2L3 L4
+ + + (1 + a2 ) ( (1 + a2 ) )
k1 k2 k3 k4
k2 = 2.97 1
φθ2 ks + 1 − 4.10 1
φθ2 kf
a21 a21
(1 + a2 ) ( (1 + a2 ) )
k3=1.16 1
θ2 ks + 1 − 1.16 1
θ2 kf
a12 a21
(1 + a2 ) ( (1 + a2 ) )
k4=2.08 1
φθ2 ks + 1 − 7.52 1
φθ2 kf
a21 a21
ks: Solid phase thermal conductivity of PCM；kf: Liquid phase thermal conductivity of PCM；LH: Height of unit pentagonal dodecahedron; Rn: Simplified quantities；Ln: height of
each layer；n = A,B,C,D: unit cell subsection.
1∑ n
( )2
MSE = keff ,exp − keff ,pre (3) Table 4
n i=1 Thermal Conductivities of some commonly used PCM and nanoparticle.
Materials Thermal conductivity(W/m.K) Reference
and the relative deviation (RD) is calculated as
⃒ ⃒ Phase change materials
⃒keff ,pre − keff ,exp ⃒ RT25(Paraffin wax) 0.25 [75]
RD = ⃒⃒ ⃒
⃒ (4)
keff ,exp Sebacic acid 0.26 [76]
D-Mannitol 1.308 [77]
In addition to the above-mentioned prediction model of effective Octadecane 0.17 [78]
thermal conductivity derived by analyzing metal foam pores, ligaments, Erythritol 0.73 [79]
and thermal conductivity of filled phase change materials, Yao et al.
[66] also proposed a new prediction model of effective thermal con Nanoparticles
ductivity of high porosity open-cell metal foam by volume averaging and Silver nanoparticle (Ag) 429 [80]
Copper nanoparticle (Cu) 400 [81]
Fourier's heat transfer to law, and validated their model with experi
Titanium dioxide (TiO2) 8.4 [81]
mental data of copper foam saturated with water, air, and paraffin. Expanded graphite (EG) 200 [82]
Carbon nanotube (CNT) 3000 [83]
3. Methods for improving the thermal conductivity of phase Graphene 3000 [84]
change materials
scattering and thus promotes heat transfer, and the effect of NPCM is
3.1. Nanoparticle dispersion into phase change materials enhanced with the increase of nanoparticle mass fraction and temper
ature [40]. However, the increase in the thermal conductivity of PCM
Recently, the application of nanocomposite phase change materials decreases as the concentration of nanoparticles gradually increases to a
(NPCM) in energy storage systems has emerged as a promising approach certain level due to the agglomeration effect that occurs when the
[67], because NPCM meets our practical applications in various fields number of nanoparticles is too large, resulting in a decrease in disper
more than pure PCM [68–72]. The thermal conductivity of NPCM is sion. The addition of appropriate surfactants (SAA) to PCM can improve
higher than that of pure PCM, partly because the thermal conductivity of these problems [85].
the nanomaterial itself is also much higher than that of PCM, as shown in
Table 4. There are many types of nanomaterials, such as carbon-based 3.1.1. Carbon based nanomaterials
nanomaterials, metal-based nanomaterials, etc. Carbon-based nano Typical carbon-based nanomaterials (CBM) carbon nanotubes,
materials have stronger thermal conductivity compared to metal-based graphite, and graphene have thermal conductivity almost five times
nanomaterials [73]. higher than metals, and with the development of emerging technologies
Nanoparticles can be divided into organic nanoparticles and inor carbon derivatives have become the first choice for enhancing the
ganic nanoparticles. The addition of inorganic nanoparticles has a better thermal conductivity of PCM [86]. The magnitude of the increase in
effect on the thermophysical properties of phase change materials thermal conductivity by adding different CBMs to different PCMs is
compared to organic nanoparticles. In contrast, organic nanoparticles different, as shown in Table 5. CBM can be divided into one-dimensional
are non-corrosive and therefore may be the best alternative for adding to (1D), two-dimensional (2D) and three-dimensional (3D) carbon-based
corrosive salt hydrates [74]. materials, as shown in Fig. 8. 1D CBM can be better embedded in
From Section 2.1.2, we can know the microscopic mechanism of phase change materials. The thermal resistance between 2D CBM and
NPCM - the nanosphere induced by nanoparticles reduces the phonon
7
Table 5
Thermal conductivity enhancement of PCMs by carbon-based additives.
PCM Thermal conductivity of Carbon additives Fraction The thermal conductivity of Enhancement in thermal Reference
PCM (W/m K) CPCM(W/m K) conductivity (%)
RT25(Paraffin wax) 0.260 CBNP 1 wt% 0.323 24.2 [75]

Soy Wax 0.324 Carbon nanofiber & 10 wt% 0.469 & 0.403 44.8 & 24.4 [88]
CNTs
OAD(Octadecylamine) 0.330 GF 15 wt% 0.725 120 [89]
Palmitic acid matrix 0.220 MWCNT 1 wt% 0.330 50 [90]
CaCl2.6H2O 0.560 Reduced GO 0.18 wt 1.008 80 [91]
%
Na2CO3.10H2O/ 0.688 Hydrothermal carbon 1.5 wt% 0.990 44 [92]
Na2HPO4.12H2O (40:60) (HTC)
Paraffin wax 0.29 rGOS 25 mg/ 0.87 200 [93]
ml
Paraffin 0.260 EG 10 wt% 3.999 1438 [94]
Paraffin wax 0.155 CBNP 2.5 wt% 0.364 135 [95]
&DUERQEDVHG
QDQRPDWHULDOV
' ' '
&DUERQ *UDSKHQH ([SDQGHG

&DUERQrEHU *UDSKLWH *UDSKLWHIRDP
QDQRWXEHV R[LGH JUDSKLWH
Fig. 8. Carbon based nanomaterials classification diagram.
PCM is smaller than 1D CBM and 3D CBM. The contact area between 3D conductivity. For example, when SWCNT and MWCNT were added to
CBM and CPM is increased, and 3D CBM is more suitable for PCM salt PCM, they were able to improve the maximum thermal conductivity
packaging [87]. of PCM by 56.98 % and 50.05 %, respectively [97].
If the nanomaterials are to be maximized, the key is the amount of Graphene (Gr) is a 2D structure composed of sp2 hybridized carbon
1D, 2D and 3D dimensional nanomaterials being added to the PCM. Alex atoms, and the microstructure is shown in Fig. 9(c). Gr is only the
Stonehouse et al. [96] found that the thermal conductivity of 3D carbon thickness of one carbon atom and there is flexibility in the inter
nano phase change materials can be enhanced by >300 % at low mass connected carbon atoms [98]. The thermal conductivity of Gr/paraffin
fractions (<5 %) and that 3D carbon nanomaterials show a positive composites is higher than that of CNT/paraffin composites with the
linear relationship between mass fraction and TCE. Among the com same filler mass fraction because of the excellent thermal and phonon
posites with high quality components, 1D and 2D have the highest vibration conductivity of the 2D structure of Gr, e.g. CNT has a higher
thermal conductivity. thermal resistance than Gr [99]. Parameters such as specific heat ca
Carbon nanotubes (CNTs) are typical 1D CBMs, and the two most pacity, density and viscosity of Gr also have a relatively large impact on
applied types of carbon nanotubes in existing research are single-walled the thermal conductivity. Elsaid et al. [100] addressed the problems
carbon nanotubes (SWCNT) and multi-walled carbon nanotubes faced by graphene-based nanofluids (NF) and suggested that because of
(MWCNT). From (a) and (b) of Fig. 9, it can be seen that the micro the lower specific heat capacity, higher density and viscosity based on
structures of SWCNT and MWCNT are different, so there is a difference Gr-based NF, the volume fraction must be well optimized in the prepa
in the extent to which adding to the same PCM improves their thermal ration of this material to withstand the increase in density and viscosity
Fig. 9. Carbon nanomaterial microstructures by SEM [97].
8
to obtain a higher thermal conductivity. to magnesium nitrate hexahydrate (an inorganic salt hydrate PCM) and
Expanded graphite (MEG), a typical 3D CBM, is of great importance found that the addition of nanoparticles not only improved the thermal
in improving the thermal conductivity of PCM. MEG is suitable for conductivity, the It also eliminated the subcooling phenomenon while
improving inorganic PCM as well as inorganic PCM. For example, maintaining the latent heat capacity. The analysis of the experimental
Shaofei Wu et al. [101] added modified potassium aluminum sulfate results shows that the thermal conductivity of NPCM is increased by
dodecahydrate (MAPSD) as PCM to MEG and found that the composite 147.5 %, 62.5 %, 55 % and 45 % by adding 0.5 wt% of TiO2, ZnO, Fe2O3
samples with MEG addition had good heat transfer properties and higher and SiO2, respectively.
thermal conductivity. The best thermal conductivity of the MEG/APSD
composite for a sample density of 900 kg/m3 and MEG content of 20 wt 3.2. Foam embedded phase change materials
% is shown in Fig. 10. Yu et al. [102] studied paraffin/expanded
graphite (PCM/MEG) composite phase change materials and found that Compared to the nanoparticles that can improve the thermal con
the thermal conductivity of CM/MEG increased with the increase of ductivity of PCM as described in Section 3.1, embedding the foam in
MEG content and bulk density. PCM not only improves the thermal conductivity more strongly, but also
has no stability problems and alleviates the generation of voids inside
3.1.2. Metal based nanomaterials the PCM [114,115]. The improvement of thermal conductivity by foam
Metal based nanomaterials can be broadly classified into two types of embedded in PCM depends mainly on parameters such as foam material,
nanomaterials, pure metal and metal oxide, which improve the thermal foam porosity, pore size, and density of pores. This paper briefly dis
conductivity of different PCMs, as shown in Table 6. cusses the more widely used metal and graphite foams.
The thermal conductivity of the metal itself is very large, with silver
(Ag) having the highest thermal conductivity (about 429 W/m.K), fol 3.2.1. Metal foam
lowed by copper (Cu). Also Ag has higher thermal conductivity than Metal Foam (MF) as the name implies is that the foam material is
metal oxides, as Harikrishnan et al. [109] used 0.5 wt% of Al2O3, SiO2, metal. From Section 3.1.2, it can be seen that different metals have
CuO, and Ag as nanomaterials and myristic acid as phase change ma different thermal conductivity, so proper selection of metal foam is
terial, and not only confirmed that the addition of metal based nano needed to improve the thermal conductivity of PCM. For example,
materials can enhance the thermal conductivity of myristic acid, but also Chaoming Wang et al. [116] found that the thermal conductivity could
Ag can make myristic acid obtain better performance, as shown in be increased by a maximum of 4.86 times when nickel foam was
Fig. 11. Ag is also able to act with other metal oxide nanomaterials in embedded in PCM compared to pure cetyl palmitate.
PCM, and Dhivya et al. [110] significantly enhanced the thermal con Among the parameters affecting the thermal conductivity of PCM-
ductivity in oleic-myristic acid eutectic PCM microcapsules with high MFs the porosity and pore density of MF are the most important pa
weight percentage of Ag-doped ZnO nanomaterials. rameters [117]. Open-cell metal foams can be divided into two types:
Although Ag has good thermal conductivity, it is relatively expensive high porosity, with porosity above 85 %; low porosity, with porosity
and highly susceptible to oxidation in air, so domestic researchers usu between 50 % and 85 % [118]. Regarding the porosity of MF, most
ally choose other metals such as Cu as nanomaterials to improve thermal national and international researchers have shown that lower porosity
conductivity for PCMs that do not require too high thermal conductivity. leads to higher thermal conductivity [114,119]. However, Hongyang Li
For example, cut copper fibers can greatly improve the thermal con et al. [120] found that MF inhibits the Rayleigh-B'enard convection of
ductivity of lithium-ion batteries using paraffin wax as PCM [111]. liquid PCM when the PCM is in the melting process of the phase tran
Xinghua Zheng et al. [112] studied the interfacial thermal conductivities sition, and the smaller the porosity of the MF, the stronger the inhibition
(ITCs) of triplet metals (Cu, Ni, Al) and PCMs and found that Cu/PCMs of this convection, which affects the thermal conductivity of PCM-MFs,
< Ni/PCMs < Al/PCMs, which is due to the dominant role of lattice as also verified in Section 2.1.1 of this paper.
vibrations in the z-direction and the mismatch at the metal/PCMs In general, the larger the pore density (ppi) of MF the weaker the
interface, as shown in Fig. 12. natural convection and overall heat transfer of the composite phase
For metal oxide nanoparticles to enhance the thermal conductivity of change material, but recently Sheng Huang et al. [121] found that when
PCM, Gupta et al. [113] added 0.5 wt% titanium dioxide (TiO2), zinc the tilt angle is 90◦ and the Rayleigh number is 4.11E+7, the metal foam
oxide (ZnO), iron oxide (Fe2O3), and silicon dioxide (SiO2), respectively, with higher pore density or smaller pore size has lower permeability,
resulting in a 50ppi composite PCM natural convection is suppressed
throughout the melting process, which reduces the heat flow to the top
of the vessel. Although the total melting time is more than 10ppi, it is
6.25 % less than 25ppi melting time, as shown in Fig. 13.
3.2.2. Graphite foam

Graphite foam is a 3D high thermal conductivity material, and the
microstructure is shown in Fig. 14. As early as 2008, researchers pro
posed to apply it to energy storage materials in space and on the ground
[122], and in recent years it has been widely used in various fields
[123–125]. Graphite foam is of great interest because of its excellent
properties such as high thermal conductivity and very high melting
point (4125 ◦ C).
Heyao Zhang et al. [126] prepared graphite foam/erythritol phase
change material and found that the thermal conductivity of the com
posite PCM increased from 40.52 W/(m.K) to 68.71 W/(m.K) and
inhibited the supercooling of erythritol from 86.0 ◦ C to 53.2 ◦ C. Hao Lan
et al. [127] also demonstrated that the thermal conductivity of graphite
foam/PCM composite phase change material is >40 times that of pure
chlorinated PCM. Similar to metal foams, the porosity of graphite foams
Fig. 10. Experimental and theoretical thermal conductivities of the MEG/APSD can control the energy storage density and heat transfer rate of LHTES
composite PCMs [101]. [128].
9
Table 6
Thermal conductivity enhancement of PCMs by metal additives.
PCM Thermal conductivity of Metal additives Fraction The thermal conductivity of Enhancement in Thermal Reference
PCM (W/m K) CPCM(W/m K) Conductivity (%)
D-Mannitol 1.308 CuO 0.5 wt% 1.637 25.2 [77]

Na2SO4.10H2O–Na2HPO4.12H2O 0.789 α-Al2O3 4.55 % 1.278 62 [103]
PEG 0.297 Al2O3 3 wt% 0.435 46.5 [104]
MP-LA/PAN (100/100) 0.11 CNPs(Copper 1.5 wt% 0.24 118 [105]
nanowires)
1-Tetradecanol 0.320 AgNW(Ag 62.73 wt 1.460 356 [106]
nanowires) %
BaCl2.2H2O 0.6146 MgO 0.2 wt% 0.7215 17 [107]
Paraffin 0.25 Fe3O4 20 wt% 0.4 60 [108]
enhancement of the heat transfer mechanism, the external field accel

erates PCM melting by increasing the convective heat transfer mecha
nism [32,130,131], as described in Section 2.1.1. This paper summarizes
three common external fields: ultrasonic, magnetic, and mechanical
vibrations.
Ultrasonic vibration is accompanied by stirring, sound, flow, cavi
tation and oscillating fluid motion, which can effectively enhance con
duction heat transfer and convection heat transfer [32], thus improving
the thermal conductivity of PCM. Ultrasound can act directly on PCM to
improve its thermal conductivity. For example, Nan Zhang et al. [132]
used ultrasound to increase the heat transfer rate of the palmitate-
stearate eutectic mixture (PA-SA) in a cylindrical stainless steel de
vice. With the increase of ultrasonic power, the heat transfer rate of PA-
SA smelting process increased, and when the ultrasonic power was 60
W, 105 W and 150 W, the heat transfer rate was increased by 10.64 %,
23.40 % and 31.91 %, respectively. With the increase of ultrasonic time,
the heat transfer rate of PA-SA also increases. Ultrasonic waves can also
indirectly act on the nanomaterials in PCM to improve the thermal
conductivity of PCM. For example, Jeon et al. [133] found that the
thermal conductivity of expanded graphite composite PCM prepared
using ultrasonic waves was improved by about 40 % compared to the
Fig. 11. Effect of thermal cycles on the thermal conductivity [109].
common stirring method, and both the dispersion stability and latent
heat of the composite PCM were improved. Recently, Shang et al. [134]
proposed that ultrasound can indirectly improve thermal conductivity
3.3. External field acting on phase change material by exfoliating graphite nanoflakes in composite PCM into nanoparticles.
The mechanism by which the magnetic field improves the thermal
In addition to adding nanomaterials to PCM and embedding PCM in conductivity of PCM is through the control of flow and heat transfer by
foam to improve thermal conductivity from the inside, it is also possible Lorentz and Kelvin forces [135]. For example, Kohyani et al. [136]
to obtain higher thermal conductivity by acting on PCM through investigated the phase change of cyclohexane-Cu nano-PCM in the
external fields. In contrast to Sections 3.1 and 3.2, which focus on the presence of a magnetic field and found that the presence of a strong
Fig. 12. (a) The ITCs of paraffin-Cu, paraffin-Ni and paraffin-Al model systems, (b) Relative contributions of lattice vibrations in x, y, and z directions to total heat
flux for paraffin/metals model systems [112].
10
magnetic field accelerated the melting process and thus enhanced

convective heat transfer. Yubin Fan et al. [130] investigated the circular
motion of magnetic particles dispersed in liquid PCM in a heat source
under the action of a rotating magnetic field and found that the rotating
magnetic field led to forced convection in liquid PCM. The total melting
time was reduced by 22.9 % when the magnetic field speed was 20 r/
min, the particle fraction was 1 wt%, and the heating temperature was
35 ◦ C.
Mechanical vibration can effectively control the crystal growth
during the phase change process, thus improving the heat transfer
characteristics of PCM during solidification. The effect of mechanical
vibration on crystallization and heat transfer is a new field based on
experimental and simulation studies. Zhang W et al. [137] conducted a
series of experiments on the battery thermal management system of pure
paraffin and three composite phase change materials (CPCMs) with
0–20 % mass fraction of expanded graphite or graphene, and found that
proper mechanical vibration can enhance the heat transfer of CPCMs
because mechanical vibration can accelerate the diffusion and collision
of highly thermally conductive particles in CPCMs, and it was concluded
that vibration has the best cooling effect on CPCMs with 20 % amount of
expanded graphite, as shown in Fig. 15.
Fig. 13. Variations in liquid fraction throughout the melting process with
different pore densities [121].
Fig. 14. Scanning electron microscope (SEM) images of the structure of graphite foam, showing the interconnected nearly-spherical pores of micro-structure in (a)
100×, and (b) 400× magnifications [129].
Fig. 15. Battery temperature at different vibration frequencies: (a) 10 wt% graphene with 90 wt% paraffin, 5C, 2 mm, T5, and (b) 20 wt% EG with 80 wt% paraffin,
5C, 2 mm, T5 [137].
11
4. Conclusion and outlook Data availability
In order to improve the thermal conductivity of PCM, this paper Data will be made available on request.
reviews the thermal conductivity mechanism, thermal conductivity
prediction model and ways to improve the thermal conductivity of PCM References
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Journal of Energy Storage 61 (2023) 106772

Contents lists available at ScienceDirect

Journal of Energy Storage

Progress of research on phase change energy storage materials in their

Phase change materials are substances that change the state of

adsorbed a binary eutectic mixture of octanoic acid-myristic acid (OA-

management system for cooling battery has gradually become a hot

2.1.2. Phonon heat transfer mechanism

mechanism for improving the thermal conductivity of NPCM. two cases.

2.1.3. Channel heat transfer mechanism 2.2.1. Nanoparticle type

Fig. 7. Microstructure of open-cell foam: (a) the microstructure of the copper

RT25(Paraffin wax) 0.260 CBNP 1 wt% 0.323 24.2 [75]

' ' '

&DUERQ *UDSKHQH ([SDQGHG

Fig. 8. Carbon based nanomaterials classification diagram.

Fig. 9. Carbon nanomaterial microstructures by SEM [97].

3.2.2. Graphite foam

D-Mannitol 1.308 CuO 0.5 wt% 1.637 25.2 [77]

enhancement of the heat transfer mechanism, the external field accel­

magnetic field accelerated the melting process and thus enhanced

4. Conclusion and outlook Data availability

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' ' '

enhancement of the heat transfer mechanism, the external field accel