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Phase change materials for electron-triggered

Cite this: J. Mater. Chem. A, 2019, 7,
energy conversion and storage: a review
22218
Yuang Zhang,†a Malik Muhammad Umair,†a Shufen Zhang a
and Bingtao Tang *ab

Received 21st June 2019
Accepted 12th September 2019
DOI: 10.1039/c9ta06678k
rsc.li/materials-a
Phase change heat storage has the advantages of high energy storage density and small temperature
change by utilizing the phase transition characteristics of phase change materials (PCMs). It is an
effective way to improve the efficiency of heat energy utilization and heat energy management. In
particular, new PCMs with energy conversion functions can effectively realize energy conversion and
storage. In recent years, energy conversion PCMs have played an important role in energy utilization and
attracted great attention. In this review, we reported the recent progress in different energy conversion
PCMs, including electric-thermal PCMs, electromagnetic-thermal conversion PCMs, photo-thermal
conversion PCMs, and photo-thermal conversion PCMs in solar thermoelectric generation. The core of
the abovementioned conversions lies in the heat release caused by electron motion or electron
transition. This process involved triggering energy conversion at the electronic level. Therefore, herein,
we aimed to comprehensively review the current development and performances of the
abovementioned energy conversion PCMs, summarize the electron-triggered energy conversion
mechanism, and suggest directions for further improvement.

utilization, energy needs to be converted or stored according to

Introduction
Energy is an important material foundation of human society.
Various energy sources are available, and many new types of
energy have begun to meet the needs of human beings through
continuous development and research.1–3 During energy
a
State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian
116024, PR China. E-mail: tangbt@dlut.edu.cn
b
Eco-chemical Engineering Cooperative Innovation Center of Shandong, Qingdao
University of Science & Technology, Qingdao 266042, PR China. E-mail: tangbt@
dlut.edu.cn
† These authors contribute equally to this article.
actual requirements. For instance, solar cells can convert solar
energy to electricity and store it, which can solve the strong
timeliness problem of the supply and demand of solar energy.4,5
Thus, the energy storage technology is as important as devel-
oping new energy sources.
Electrical energy storage,6 electrochemical energy storage,7,8
chemical energy storage,9 and thermal energy storage (TES) are
some of the many available approaches for storing energy.10,11
Among them, the TES technology has broad application pros-
pects in solar energy utilization, “peak-load shiing” of electric
power, recovery and utilization of waste heat, and energy
conservation of building heating. Phase change materials

Yuang Zhang received her BSc Malik Muhammad Umair is

degree in Dalian University of currently a PhD candidate under
Technology, and now is the supervision of Prof. Bingtao
currently a PhD candidate under Tang at Dalian University of
the supervision of Prof. Bingtao Technology. His research inter-
Tang. She was awarded ests include the synthesis of
a National Scholarship by the multifunctional phase change
Ministry of Education of the materials for thermal energy
People's Republic of China in storage.
2017. Her current research
interests focus on the energy
conversion phase change mate-
rials and solar thermoelectric
generation.

22218 | J. Mater. Chem. A, 2019, 7, 22218–22228 This journal is © The Royal Society of Chemistry 2019

Review
(PCMs) can store and release large amounts of latent heat
energy within a slight temperature change through a phase
transition, which have the most potential for use in thermal
storage. Based on this property, PCMs have been widely
researched in thermal management and storage.12–16 Worldwide
scholars are committed to introduce other energy conversion
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media into PCMs and to obtain phase change composite
materials with energy conversion and storage functions.
Energy conversion PCMs have attracted considerable atten-
tion. To the best of our knowledge, many review articles have
summarized composite PCMs, such as PCMs in buildings,17,18
thermal conductivity enhancement PCMs,19,20 carbon-based
PCMs,21,22 nanoporous shape-stabilized PCMs,23 and the proper-
ties and commercialization of PCMs.24 However, a comprehen-
sive overview of energy conversion PCMs and their conversion
mechanism has not been presented. Therefore, we tried to
provide a comprehensive perspective of the recent advances in
energy conversion PCMs from the perspective of conversion
mechanism, including electric-thermal PCMs, electromagnetic-
thermal conversion PCMs, photo-thermal conversion PCMs,
and photo-thermal conversion PCMs in solar thermoelectric
generation. The core of the abovementioned conversions lies in
the heat release caused by electron motion or electron transition.
The process involved triggering energy conversion at the elec-
tronic level. Thus, we classied and named them as electron-
triggered energy conversion PCMs. Based on summarizing
energy conversion PCMs, this paper aims to deeply understand
their electron-triggered energy conversion mechanism, thereby
providing a theoretical basis for the construction of efficient
energy conversion PCMs and summarizing current issues and
future research directions.
2 Electron-triggered energy
conversion PCMs
2.1 Electric-thermal conversion PCMs
Considering the insulating properties of PCMs, researchers
have focused on designing electrically conductive supporting
materials suitable for achieving electric-driven and form-stable
phase changes in PCMs. Electric-thermal energy conversion and
Shufen Zhang is currently
a Professor at Dalian University
of Technology. She is a Distin-
guished Professor of Changjiang
Scholar, and winner of the
National Science Fund for
Distinguished Young Scholars.
Her research interests include
dye chemistry, photochemistry,
biomass materials, and
photonic crystal.
This journal is © The Royal Society of Chemistry 2019
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Journal of Materials Chemistry A
storage have undoubtedly widened the application scope of
PCMs, particularly in the thermal management of electronic
devices. The basic mechanism underlying electric-thermal
conversion is as follows: moving electrons collide with other
molecules or groups to generate Joule heat, which is released
when electric current ows through a conductive PCM
composite (Fig. 1b).25 The resistive heat is absorbed by the
PCMs and is eventually stored as latent heat. The conventional
materials used for Joule heating are metals and metal alloys.
However, carbon materials, such as carbon nanotubes (CNTs),
graphene, and graphite are found to be efficient alternatives.
CNT sponges were rst introduced by Zou and Cao's group as
porous structures used to encapsulate paraffin via the inltra-
tion method.26 Under an applied voltage bias of 1.75 V, the
CNT–paraffin composite achieved an electro-thermal conver-
sion efficiency of 52.5%. In the subsequent study, CNT arrays
Fig. 1 Electronic-trigger energy conversion mechanism diagram of
electromagnetic-thermal conversion PCMs (a), electric-thermal PCMs
(b), and photo-thermal conversion PCMs (c).
Bingtao Tang is currently
a Professor at Dalian University
of Technology. He received his
Doctorate at Dalian University
of Technology in 2005, and
became a Professor in 2016. His
research interests include energy
conversion and storage, dyestuff
chemistry and photochemistry,
micro/nano interface and struc-
tural color. During his career,
his research has resulted in 100
papers and 18 patents.
J. Mater. Chem. A, 2019, 7, 22218–22228 | 22219

Journal of Materials Chemistry A
(CNTA) composed of ordered anisotropic structures were inl-
trated with melted n-eicosane (C-20) (Fig. 2a).27 The areal
density of the fabricated CNT arrays was modulated by direct
lateral compression. The distinctive property of compression
increased the alignment and the contact between the PCM and
the CNT arrays. Thus, the heat transfer increased, and the bulk
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resistance decreased in the composites. Consequently, the
higher compression (40%) sample required a lower voltage (1 V)
to trigger the phase change compared with the uncompressed
samples and previously reported CNT sponges with a disor-
dered structure (Fig. 2b). A CNT array-eicosane composite ach-
ieved 74.7% electro-thermal conversion efficiency at a voltage
bias of 1.3 V. Recently, Aab et al.28 reported a exible poly-
urethane (PU)-CNT composite with an anisotropic structure.
The freestanding and macroporous CNT sponge was synthe-
sized via the CVD method. A rectangular sample of CNT sponge
was immersed in a DMF solution of PU and later vacuum-dried
to obtain a solid–solid PCM composite. The electro-thermal
conversion efficiency of the polyurethane PU-CNT composite
reached 94% under an applied voltage of 2 V. The shape
recovery aer the application of 30% strain suggested that the
PU-CNTs were sufficiently exible for device fabrication in
biomedical applications.
Fig. 2 (a) Schematic illustration of the CNTA-C20 composite struc-
ture and its fabrication. (b) Temperature–time curves of the CNTA-
C20-c40% composite under 1.0–1.3 V. Adapted with permission from
ref. 27, Copyright 2013, American Chemical Society. SEM images of
AN-GA in the axial direction (c) and radial direction (d). (e) Tempera-
ture–time curves of AN-GA-paraffin under 0.5–3.0 V. Reproduced
with permission from ref. 29, Copyright 2016, The Royal Society of
Chemistry. (f) Illustration of the composition and structure of the
functional protective wear product. (g) Temperature–time relationship
of the electro-driven PU/graphite foam composite under 1.5–1.8 V.
Reproduced from ref. 34 with permission from Elsevier.
22220 | J. Mater. Chem. A, 2019, 7, 22218–22228
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Graphene aerogels with an anisotropic structure are of great
interest in the fabrication of electric-driven PCMs because of
their remarkable conductivity and structural stability. Li et al.29
designed an anisotropic graphene aerogel (AN-GA) by employ-
ing gaseous HCl to in situ solidify graphene oxide (GO) liquid
crystals, followed by chemical reduction, critical drying, and
annealing treatments. The thermal and electrical conductivity
of the graphene aerogel/paraffin composite was higher in the
axial direction compared with the radial direction due to the
alignment of the graphene sheets (Fig. 2c and d, respectively).
Consequently, the anisotropic PCM composites possessed
a fast-response electro-thermal effect and achieved an electro-
thermal conversion efficiency of 85.4% at 3 V (Fig. 2e). In
another study by Guo et al.,30 the 3D interconnected network of
CNTs/GO was inltrated with PEG-1000. The electro-thermal
conversion efficiency of the obtained PCM composite was
approximately 70% under 6.6 V, which was reduced to 63%
under a higher voltage (7.0 V) due to convection heat loss to the
air. In a study by Zhou et al.,31 a hybrid halloysite nanotube/
graphene aerogel supporting skeleton was fabricated and
inltrated with PU. The halloysite nanotubes improved the
reduction degree of the graphene aerogel and the latent heat
storage of PCM composites through the heterogeneous nucle-
ation effect. However, the electro-thermal conversion efficiency
of the PCM composite was 66.3% under 10 V. The above-
mentioned studies clearly show that the anisotropic structure of
CNTs and graphene-supported PCM composites are contrib-
uting factors to high electric-thermal conversion efficiency.
Some cheap carbon materials also have electric-thermal
properties. Maleki and Beitollahi32 prepared a 3D inter-
connected porous carbon foam from polyacrylonitrile that
could load organic PCMs and presented high electric-thermal
efficiency (up to 74%).
Graphite foams are widely used supporting skeletons for
loading PCMs due to their ordered porous structure, high
conductivity, low density, and cost effectiveness. Zou's group
reported a systematic study on the performance of electric-
driven PU as a solid–solid PCM embedded in graphite foam.
In their study, PU was synthesized via inltration in graphite
foam, and a later study involved the in situ PU polymerization
within the graphite foam.33 The results of both studies showed
the electric-thermal conversion efficiency of PU/graphite foam
composites of approximately 80–85% at 1.2–1.8 V. Another
study also achieved a signicantly reduced supercooling degree
in a PU solid–solid PCM.34 In addition, the application of
a functional protective wear for cold environments was
demonstrated by embedding the electric-driven PU/graphite
foam composite (15 cm
10 cm
2 cm) in a winter coat
(Fig. 2f and g). According to the test results, the heat discharg-
ing was prolonged two times more in functional wear than in
normal wear aer battery-assisted charging. Thus, the electric-
driven PCM provided satisfactory protection against cold by
keeping the temperature in the comfort range for a long period
of time.
Porous carbon derived from biomass sources are reported as
efficient supporting materials for encapsulating PCMs. The
sustainable raw materials, impressive thermophysical
This journal is © The Royal Society of Chemistry 2019

Review
properties, and high absorption capacity of porous carbon can
be utilized in large-scale PCM applications, such as building
materials. Li et al.35 prepared a carbon aerogel via the hydro-
thermal carbonization of water melons, and paraffin was inl-
trated to obtain a PCM composite with an electrical conductivity
of 3.4 S m1 and electric-thermal conversion efficiency of 71% at
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15 V.
The working voltage and efficiency are two key factors of
electric-thermal conversion PCMs. Hence, while maintaining
high electric-thermal conversion efficiency, reducing the
working voltage to improve their application security will be the
focus of attention in the future.
2.2 Electromagnetic-thermal conversion PCMs
Periodic electron motion (alternating current) can produce
alternating magnetic elds (AMF), in which superparamagnetic
materials can release heat through Néel relaxation or Brownian
relaxation (Fig. 1a).36,37 Based on this property of super-
paramagnetic materials, researchers have combined these
materials with PCMs to prepare electromagnetic-thermal
conversion PCMs.
Nano Fe3O4 is the most common electromagnetic-thermal
ller.38–40 Wang et al.41 introduced a Fe3O4-functionalized gra-
phene nanosheets (Fe3O4–GNS) into a PU PCM. Fe3O4–GNS
endowed the Fe3O4–GNS/PCM with magnetic and sunlight dual-
driven energy conversion and storage performances (Fig. 3a).
Fe3O4–GNS/PCM could convert magnetic energy to thermal
energy and store it through phase transition under AMF
because of the superparamagnetism of the Fe3O4 nanoparticles
(Fig. 3b). A high additive amount of Fe3O4–GNS resulted in
a high heating rate. In addition, the magnetic-thermal energy
Fig. 3 (a) Diagram of magnetic-and sunlight-thermal energy
conversion and storage. (b) Electromagnetic-thermal energy conver-
sion and thermal storage curves of the Fe3O4–GNS/PCM composites
under AMF (1.36 MHz, 500 A m1). (c) Electromagnetic-thermal energy
storage efficiencies of the Fe3O4–GNS/PCM composites. Reproduced
with permission from ref. 41, Copyright 2017, The Royal Society of
Chemistry.
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Journal of Materials Chemistry A
storage efficiencies increased from 18.7% to 41.7% with an
increase in the Fe3O4–GNS content (Fig. 3c). In another study,
Fan et al.42 prepared an SiO2 gel network to load polyethylene
glycol (PEG) and Fe3O4 nanoparticles through the in situ sol–gel
method. The prepared Fe3O4/PEG/SiO2 composites exhibited
shape stability, electromagnetic-thermal conversion, and phase
change energy storage performances simultaneously.
PCMs, due to their relatively stable temperature during the
phase change, have been regarded as ideal medium materials in
the medical eld, such as thermotherapy and drug release
systems. Thus, the electromagnetic-thermal conversion of
PCMs is mainly applied in the elds of magnetic thermotherapy
and magnetically triggered drug delivery. In addition, when
electromagnetic-thermal conversion PCMs are applied in
human disease treatment, the most important aspect is to
regulate the phase change temperature in the range of 41–47  C,
which can release drugs or kill pathological cells without
causing irreversible damage to normal cells.43
Wang et al.43 designed an extracorporeal magnetic thermo-
therapy material (Fe3O4@SiO2/PCM) by introducing super-
paramagnetic Fe3O4@SiO2 core–shell colloids into a phase
change matrix (Fig. 4a). The Fe3O4@SiO2/PCM could be driven
in AMF and maintained a temperature range of 41–47  C for
a long time (Fig. 4b). The temperature control efficiency of
Fe3O4@SiO2/PCM reached up to 60.2%.
Ghosh and co-workers44 capped Fe3O4 magnetic nano-
particles with oleic acid (OA) or PEG and explored their
magnetic hyperthermia applications in cancer therapy. They
discovered that human breast cancer cells showed a 35%
decrease in viability aer Fe3O4-OA treatment compared with
the untreated control.
Electromagnetic-thermal conversion PCMs can be utilized in
drug delivery by using an external magnetic eld to control the
release of drugs in the body to achieve accurate drug delivery.
Zhang et al.45 reported a new drug release system consisting of
Fe3O4 nanoparticles, 1-tetradecanol (PCM), PEG, and doxoru-
bicin (DOX). The Fe3O4@PCM/PEG/DOX system achieved nearly
zero release in body temperature and could be driven by both
NIR laser irradiation and AMF. Under AMF, the Fe3O4 nano-
particles rapidly underwent electromagnetic-thermal trans-
formation. When the temperature reached the phase change
temperature, the drug was released. Meanwhile, due to the
phase change properties of the PCM, the system temperature
was guaranteed to be within 42  C during release, which does
not damage the human body.
Li et al.46 developed an anticancer drug delivery system for
thermo-chemotherapy based on PCM and hollow magnetic
nanoparticles (HMNPs). HMNP@PCM@DOX could quickly
generate heat under AMF and reached the temperature for
cancer hyperthermia (>42  C) within 30 min (Fig. 4c). The tumor
temperature in mice increased in vivo aer treatment (Fig. 4d).
Simultaneously, anticancer drugs were released during hyper-
thermia. Combined with hyperthermia and chemotherapy, the
tumor experiment in mice proved that the thermo-
chemotherapy method of this system had an obvious inhibi-
tory effect on tumors (Fig. 4e).
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Journal of Materials Chemistry A Review

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Fig. 4 (a) Schematic illustration of the electromagnetic-thermal energy conversion of Fe3O4@SiO2/PCM. (b) Temperature curves of Fe3O4@-
SiO2/PCM under an AMF (1.10 MHz, 700 A m1). Reproduced from ref. 43 with permission from Elsevier. (c) Infrared thermographic images of
centrifuge tubes containing HMNP@PCM@DOX solution under an AMF (300 A, 200 kHz, 4 kW). (d) Tumor temperatures change with different
treatments. (e) Magnetic resonance images of nude mice obtained at day 0 before and after injection and day 7 after treatment. Reproduced with
permission from ref. 46, Copyright 2015, The Royal Society of Chemistry.

It is evident from these works that electromagnetic-thermal
conversion PCMs have great application prospects for drug
release and thermotherapy. However, further research is
needed on the targeted therapy and toxicity of electromagnetic-
thermal conversion PCMs.
2.3 Photo-thermal conversion PCMs
Among the various energy sources, solar energy is identied as
one of the most potential renewable energy sources because it is
abundant, universal, sustainable, and clean.47,48 Therefore,
photo-thermal conversion PCMs are the most frequently
studied among the energy conversion PCMs. The basic mech-
anism of photo-thermal conversion is that light can excite
photo-thermal llers, thereby making electrons jump to the
excited state. Then, the excited electrons will release energy
back to the ground state by nonradiative relaxation, energy
transfer, or quenching.49,50 All of the above relaxation modes are
accompanied by heat release (Fig. 1c). Table 1 shows the
thermal properties and photo-thermal performances of repre-
sentative photo-thermal conversion PCMs with various photo-
thermal llers, and more details will be discussed later in this
review.
The key factor of photo-thermal conversion PCMs is the
photoabsorber and converter. Dyes are a potential and
outstanding photoabsorbers and converters. In recent years,
our group conducted several studies and synthesized a series of
light-driven dye-PCMs.51–55 Our group also pioneered the intro-
duction of dyes into PCMs to prepare photo-thermal PCMs.
Three dyes containing chlorosulfonyl or active chlorine and
functionalized MPEG were linked through polyethylene poly-
amine and formed organic photo-thermal conversion materials
(OPTCM).55 The dyes and PCMs are reactive agents of compos-
ites and act as light capture and thermal energy storage
modules, respectively (Fig. 5a). The photo-thermal conversion
mechanism was also conjectured. The dye molecules absorb
photons and reach the excited state. Then, they rapidly transi-
tion to the ground state by the thermal release approach (non-
radiative relaxation), including vibration relaxation, internal
conversion, and intersystem crossing (Fig. 5b). The photo-
thermal conversion and storage efficiency (h) can be close to
94%. Furthermore, we polymerized a dye and PEG to form
a polymer skeleton (dye-PU) and then loaded hexadecanol to
obtain a form-stable light-driven phase change composite with
high latent heat.52 Hexadecanol/dye-PU composites have high
phase change enthalpies (Fig. 5c) and photo-thermal conver-
sion properties due to the phase transition properties and light
absorption capacity of their supporting skeleton. Furthermore,
no leakage is observed above the phase change temperature
(Fig. 5d) because of the excellent supporting characteristics of
dye-PU.

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Review Journal of Materials Chemistry A

Table 1 Thermal properties and photo-thermal performances of photo-thermal conversion PCMs

Photo-thermal
Photo-thermal Latent Optical power conversion
ller Melting point heat intensity and storage efficiency
Sample content (wt%) ( C) (J g1) (mW cm2) (%) Reference

MPEG-polyamine-dye-TDI (yellow and — 58.8 128.7 255.1 94.4 51

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red)
Hexadecanol (63.8%)/dye-PU — 39.6/50.3 229.5 75.5 — 52
Dye-PU PCM — 53.4 112.9 300.0 95.0 77
PEG-co-dye (ma) — 65.9 178.7 61.2 93.7 54
MPEG-polyamine-dye (yellow) — — 103.2 61.2 97.3 55
RGO/PU PCMs 9.1 55.9 107.2 100.0 78.7 57
CF/PEG/SiO2 5.0 61.4 132.4 189.8 — 58
Palmitic acid/OA-rGO 2.0 64.8 181.9 111.6 — 61
Paraffin wax/graphene foam — 56.8 153.1 — 89.0 62
PEG/cellulose/graphene aerogel 5.3 63.0 156.1 — — 64
Carbon aerogel/octadecanol 24.1 — 175.0 100.0 — 65
Ti4O7/PEG/SiO2 3.0 59.8 129.8 — — 72
Paraffin@SiO2/Ti4O7 3.0 52.2 122.4 100.0 85.4 73
Paraffin/graphene foam 3.0 60.8 200.0 150.0 79.9 76
PEG/Ag-GNS 8.0 60.3 166.1 120.0 92.0 69
PEG/Ti3C2Tx 20.0 61.3 157.9 128.6 94.2 75
PEG/GO/BN 20.0 65.4 145.6 100.0 83.8 78
PEG/BN/GNP 1.0 63.8 122.2 100.0 72.7 79

harvesting properties through a solar water heating experiment

Fig. 5 (a) Schematic diagram of OPTCM light-to-heat conversion and
energy storage. (b) Photo-thermal conversion mechanism of dye-
PCMs. Reproduced with permission from ref. 55, Copyright 2012, The
Royal Society of Chemistry. (c) DSC curves of dye-PU, hexadecanol
and hexadecanol/dye-PU composite. (d) Digital photographs of hex-
adecanol/dye-PU composite, hexadecanol and dye-PU at different
temperatures. Reproduced with permission from ref. 52, Copyright
2015, Elsevier.
Carbon materials, especially nanocarbon materials, are
usually chosen as the photo absorber and converter because of
their strong light absorption, physical properties, and very high
thermal conductivity.21 Carbon materials release heat mainly
through the electron phonon coupling mechanism.
A. Kardam and co-workers56 utilized nanographite (NG) and
CNT as nanollers to for a composite with inorganic PCM
Mg(NO3)2$6H2O and investigated its heat transfer rate and solar
(Fig. 6a). The experimental observations showed that the system
with the NG–PCM composite reached a high temperature much
faster than that with the pristine PCM (Fig. 6b). This condition
was attributed to the fast thermal diffusion of the uniformly
dispersed nanocarbon materials. Furthermore, the authors
found that CNTs performed better than NGs in harvesting,
converting, and storing the broad spectrum solar energy. Their
good light absorption is believed to stem from the van Hove
transitions within or between the p-bands of CNTs.
Zhou et al.57 prepared crosslinked PU-based PCMs with
reduced graphene oxide (RGPCMs) using GO and PEG as
working parts and hexamethylene diisocyanate biuret (HDIB) as
a crosslinking agent. Thus, GO sheets reacted with HDIB to
form a crosslinking network and were reduced simultaneously.
The advantage of this strategy is that the nal products will
form 3D crosslinking networks regardless of the RGO content.
The RGO could serve as a crosslinking skeleton at high content
and act as crosslinking knots at low content (Fig. 6c). The
fantastic structure not only endowed the RGPCMs with an
excellent form-stable performance but also outstanding photo-
thermal conversion properties. The temperature of the
RGPCMs increased rapidly under solar radiation due to the
excellent light absorbing property of RGO. In addition, the
photo-thermal conversion properties were proportional to the
RGO content (Fig. 6d). The photo-thermal conversion and
storage efficiency (h) of the RGPCMs reached 78.7% with
9.1 wt% RGO.
Our group58–60 reported a series of nano-carbon containing
light-driven PCMs. In one of our studies, carbon ber (CF) was
utilized as a light-driven ller and introduced to a PEG/silica
(SiO2) system through a sol–gel process.58 The absorption
properties of CF and CF/PEG/SiO2 were investigated through

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Journal of Materials Chemistry A Review

absorbed solar energy. Thus, its temperature increased and

reached the phase change platform (Fig. 7e), whereas pure
octadecanol could not reach its phase change temperature and
realize solar energy storage due to its lack of light absorption.
Nevertheless, light absorption capacity and thermal radia-
tion determine the photo-thermal utilization efficiency.
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Although carbon materials have high light absorption capacity,

their high emissivity values (usually over 0.8)66 lead to a low
photo-thermal utilization efficiency.67,68 Thus, further
improving the photo-thermal utilization efficiency of photo-
thermal conversion PCMs is still a research hotspot.
Further improvement of the light absorption ability of
carbon materials is an effective solution. Some metal nano-
particles can enhance thermal generation by localized surface
plasmon resonances (LSPR) because they have many mobile
electrons for the conversion of heat. The LSPR is a unique
optical phenomenon that occurs in some metallic structures,
Fig. 6 (a) Schematic diagram of solar water heating experimental set- such as silver, gold, and platinum. When the frequency of
up. (b) Temperature–time of water using the solar water heating
incident light and oscillation frequency of delocalized electrons
experimental setup. Reproduced with permission from ref. 56, Copy-
right 2015, The Royal Society of Chemistry. (c) Schematic illustration of in metals are consistent, collective excitation leads to remark-
the cross-linking network of RGPCMs with different RGO contents able heating.50 According to this mechanism, researchers have
during the phase transition process. (d) Photo-thermal conversion introduced metal nanoparticles into carbon materials to
experiment: temperature–time curves of RGPCMs under sunlight increase their photo-thermal conversion efficiency. Zhang
radiation at 100 mW cm2. Reproduced with permission from ref. 57,
et al.69 designed a novel enhanced photo-thermal conversion
Copyright 2018, Elsevier.
composite by introducing Ag nanoparticle-functionalized gra-
phene nanosheets (Ag–GNS) into PEG (Fig. 8a). Based on the
LSPR effect of the Ag nanoparticles, the composites exhibited
solid ultraviolet-visible absorption measurement. CF demon-
improved photo-thermal and energy storage efficiency from
strated high absorption at all visible light bands. Thus, the CF/
70.8% to 92.0% (Fig. 8b). Deng and Tao's group found a new
PEG/SiO2 composites had enhanced visible-light absorption in
magnetically moving way to increase the energy harvesting
proportion to the CF content.
efficiency from the perspective of the heat transfer mecha-
Furthermore, some carbon materials can be used as sup-
nism.70,71 In one of their studies, they introduced Fe3O4@-
porting materials to obtain form-stable PCMs due to their
graphene optical absorbers into a paraffin system and
porous or layer structures.
accelerated the heat transfer through the dynamic tuning
Akhiani and his group61 reduced and functionalized GO with
distribution of Fe3O4@graphene with a magnetic eld (Fig. 8-
long chain alkylamine and oleylamine and then formed a 3D
c(iii)).70 Compared with the traditional photo-thermal conver-
structure via self-assembly with palmitic acid (PA) (Fig. 7a).
sion heat transfer approaches, as shown in Fig. 8c(i) and (ii), the
Compared with pure PA, the composites showed better perfor-
charging rate increased by 60% and 270%. The energy har-
mance in the light-to-heat conversion. Yang's group62 reported
vesting efficiency also increased by 64.3%.
a 3D hierarchical graphene foam and used it to support
Some metal oxides are also applicable photo-thermal llers.
paraffin, and the obtained composite exhibited high photo-
Ti4O7/PEG/SiO2 form-stable PCMs have been developed by Tang
thermal energy conversion and a storage efficiency of 89%.
and coworkers to improve the utilization efficiency of solar
Carbon aerogels (CA) are a type of lightweight, porous,
energy.72 They reported that the Ti4O7/PEG/SiO2 composites had
amorphous carbon nanocomposites. Their 3D porous structure
wide solar radiation absorption capacity and could effectively
make them a potential support framework for solid–liquid
harvest visible light. Li et al.73 designed new paraffin@ SiO2/
PCMs.63–65 Huang et al.65 designed a CA/octadecanol composite
Ti4O7 microcapsules, which exhibited a photo-thermal storage
PCM and investigated its shape-stability mechanism and photo-
efficiency of 85.36% with 3 wt% Ti4O7. In another work, Ni
thermal conversion performance. The CA was synthesized from
et al.74 used Cu–Cu2O as shell materials to coat phase change
glucose via sol–gel and carbonization. The SEM image of CA
paraffin wax to prepare a new type of heat transfer uid with
displays that interconnected nanoparticles form a highly
photo-thermal properties. The effective receiver efficiency of the
porous aerogel (Fig. 7c), and the N2 absorption and desorption
paraffin@Cu–Cu2O slurry reached over 90% at 40  C.
isotherms further prove the presence of micro-porosity and
Besides, an increasing number of new photo-thermal
macro-porosity (Fig. 7b). Aer octadecanol inltration, the
conversion PCMs with excellent properties have been discov-
rough nanoparticles were wrapped by octadecanol, and their
ered. Recent studies have found that as a new material, MXenes
pores were lled (Fig. 7d). The carbon aerogels also endowed
are also an excellent photo-thermal conversion agent, and their
the composites with excellent light absorption. When CA/
large specic surface area and two-dimensional structure can
octadecanol was exposed to simulated light, the composite

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 View Article Online

Review Journal of Materials Chemistry A

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Fig. 7 (a) Schematic illustration of the reduction, functionalization and self-assembly process. Reprinted with permission from ref. 61, Copyright
2015, American Chemical Society. (b) N2 absorption and desorption isotherms of the CA and CA/octadecanol composite, and inset shows the
corresponding pore size distributions. SEM images of (c) pure CA and (d) CA/octadecanol composite. (e) Illustration of the photo-thermal energy
conversion experiment and the time–temperature curves of pure octadecanol and CA/octadecanol composites under simulated solar radiation
at 50 and 100 mW cm2. Reproduced with permission from ref. 65, Copyright 2014, The Royal Society of Chemistry.

directly bind PCMs to overcome the leakage problem. The

Fig. 8 (a) Schematic illustration showing the visible light-thermal
energy conversion and storage of the Ag-GNS/PEG composites. (b)
Photo-thermal conversion curves of PEG 6000, GNS/PEG and Ag–
GNS/PEG composites under solar simulator radiation (I ¼ 120 mW
cm2). Reproduced with permission from ref. 69, Copyright 2019,
Elsevier. (c) Three photo-thermal conversion heat transfer mecha-
nisms: thermal-diffusion-based thermal charging approach (i),
photon-transport-based optical charging approach (ii) and magneti-
cally enhanced photon-transport based optical charging (iii). Repro-
duced with permission from ref. 70, Copyright 2017, Springer Nature.
photo-thermal storage efficiency can reach 94.2%.75
Photo-thermal-electric conversion is a further application of
photo-thermal conversion PCMs. Using the Seebeck effect of the
thermoelectric module, the heat energy converted from light
through photo-thermal PCMs can be further transformed into
electrical energy. Furthermore, based on the phase change
characteristic of photo-thermal PCMs, a stable output current in
a period of time can be obtained.
Zhang et al.76 reported a graphene–PCM composite based on
3D graphene foams and paraffin wax. With the combination of
photo-thermal conversion and heat storage capability, the gra-
phene–wax composite was applied in a light-driven thermo-
electric conversion system and realized sustained power
generation (Fig. 9a–d). In addition, a small fan could be driven
by the light-driven thermoelectric conversion system under
1500 W m2 light irradiation, and the fan continued to run for
10 min aer the light source was turned off (Fig. 9e). Our
group77 designed and constructed a sunlight-driven thermo-
electric system using a photo-thermal PCM (PCHSM) as the hot-
side and a phase change cool storage material (PCCSM) as the
cold-side to control the temperature (Fig. 9f). The temperature
gradient was controlled through the hot and cold-side materials
based on their phase change characteristics, and a stable output
current was obtained under sunlight (Fig. 9g). In addition,
based on several previous works, we studied the photo-thermal
conversion mechanism of dye-PCMs using femtosecond tran-
sient absorption.77 The dye molecules were excited by light.
However, the excited state was not stable. Thus, the dye

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Fig. 9 (a) Schematic diagram of the light-driven thermoelectric set-
up. Time-output voltage of the thermoelectric modules under the
simulative light source of 1500 W m2 (red) and 1000 W m2 (black) (b)
without the composite, (c) with 6.3 g composite, (d) with (solid lines)
and without the composite (dashed lines) after the light was turned off.
(e) Digital photograph showing the continuous operation of the fan
driven by the thermoelectric system with 13.5 g composite in the
absence of light. Reproduced with permission from ref. 76, Copyright
2016, The Royal Society of Chemistry. (f) Device diagram and sche-
matic diagram of energy conversion. (g) Current/temperature–time
curves for the solar-thermal-electric energy conversion experiment
under the sunlight (I ¼ 98 mW cm2). Reproduced from ref. 77 with
permission from Elsevier.
molecules went back to the ground state, and the energy was
transferred to the polymer chain by intramolecular energy
transfer. Then, the polymer chain released excess energy in the
form of heat through molecule vibrations (Fig. 9f).
Yang and his group synthesized a series of photo-thermal
phase change composites containing PEG, boron nitride
(BN), and GO or graphene and then applied them in photo-
thermal-electric conversion.78–81 Under the action of the
phase change composites, stable output currents and voltages
could be both obtained during the stage of energy storage and
energy release.
Therefore, photo-thermal-electric energy conversion
expands the applications of photo-thermal PCMs, especially in
the eld of solar thermoelectric generation. Besides improving
the optical capture and photo-thermal conversion performance
of photo-thermal PCMs, the improvement of their thermoelec-
tric efficiency and processability of their thermoelectric module
is also crucial.
3. Conclusion and outlook
In conclusion, we presented a detailed review on the current
development of different electronic-trigger energy conversion
PCMs, including electric-thermal PCMs, electromagnetic-
22226 | J. Mater. Chem. A, 2019, 7, 22218–22228
View Article Online
Review
thermal conversion PCMs, photo-thermal conversion PCMs,
and photo-thermal conversion PCMs in solar thermoelectric
generation. In particular, the electronic-trigger energy conver-
sion mechanisms summarized herein can make it easy for
readers to deeply understand the theory of energy conversion
PCMs and improve the energy conversion efficiency from the
mechanism.
In our opinion, several critical issues and research directions
worthy of further investigation are as follows:
 From the point of view of the electron collision mecha-
nism, electric-thermal conversion PCMs need electric
conductivity to allow electron ow and require resistance to
generate Joule heat. The key is nding the best balance point
to safely obtain low-voltage drive and high energy conversion
efficiency.
 Electromagnetic-thermal PCMs, which are of great signif-
icance in curing diseases and overcoming medical problems,
such as magnetic thermotherapy and magnetically triggered
drug delivery, can be used in human biotics. This aspect is
a meaningful research direction. The magnetic moment, size of
magnetic particles and targeted therapy are important issues
requiring further study.
 For photo-thermal PCMs, carbon-containing PCMs are the
most commonly used. To solve the low efficiency of carbon-
containing PCMs, introducing metal particles with LSPR
effects to increase their light absorption or change their heat
transfer mode is a very sensible approach. However, studies on
this aspect are few despite its meaningful research direction.
This topic is also a worthy research direction to explore more
new photo-thermal llers.
 For photo-thermal-electric energy conversion, in addition
to the abovementioned improvement of the properties of photo-
thermal PCMs, improving the performance of the thermoelec-
tric component and reducing the heat loss between modules are
important research directions. In addition, exibility and
portability of the system are important issues that need to be
addressed.
In summary, the development of multifunctional energy
conversion PCMs is still popular and meaningful research.
Further efforts should be made to improve the properties and
efficiencies and expand the application of energy conversion
PCMs.
Conflicts of interest
There are no conicts to declare.
Acknowledgements
This work was supported by the National Natural Science
FoundationFoudation of China (21878043, 21576039, 21421005
and U1608223), Program for Innovation Research Team in
University (IRT_13R06), the Fundamental Research Funds for
the Central Universities (DUT18ZD218), Talent Fund of Shan-
dong Collaborative Innovation Center of Eco Chemical Engi-
neering (XTCXYX04).
This journal is © The Royal Society of Chemistry 2019

Review
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