Solar Energy Materials & Solar Cells 250 (2023) 112075

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Solar Energy Materials and Solar Cells

journal homepage: www.elsevier.com/locate/solmat

Core-satellite assembly of phase-changing material microcapsules enabled

with broadband light absorption and localized surface plasmonic resonance
for effective photothermal energy harvesting
Arni M. Pornea a, b, Hern Kim b, *
a
R & D Center, Naieel Technology, Republic of Korea
b
Department of Energy Science and Technology, Environmental Waste Recycle Institute, Myongji University, Yongin, Gyeonggi-do, 17058, Republic of Korea

A R T I C L E I N F O A B S T R A C T

Keywords: To enhance the comprehensive photo-thermal energy accretion of the confined phase-changing materials
Solar thermal energy storage (EPCM), engineered plasmonic nanoparticles (PG) and photosensitizer (PDA) were assimilated and structured in
Phase changing materials (PCM) a core-satellite manner to form a highly active composite shell (DS-PDA/PG). In this communication, we devise a
Localized surface plasmonic resonance (LSPR)
heterogeneous core-satellite assembly by the conjugation of the PCMs core and PG satellite assisted by a PDA
Photothermal effect
Photothermal conversion efficiency
arresting media. The constructed core-satellite can distinctly demonstrate superior photothermal performance
compared to their respective precursor. This structural framework enunciates substantial improvement in pho­
tothermal energy conversion and heat dissipation mechanism due to the synergistic effect between the PG sat­
ellite and the PDA linker. Particularly, the heat channeling effect of PG nanoparticles onto the structured
framework due to its localized surface plasmonic resonance (LSPR) mitigation which effectively dissipates heat
to the encapsulating shell. The curated approach achieved a phase transition enthalpy of 139.20 J/g, with a
thermal discrepancy of 28.89 ± 1.21 ◦ C attaining an augmented photo to heat energy conversion efficiency of
96.95% due to wideband solar absorption and effective heat dissipation through the core-satellite assembly. The
structured consolidation of PG and PDA was recognized to be a functional strategy that reinforce substantial
improvements toward direct photo energy cultivation in an assortment of applications such as temperature
management of greenhouses, solar water heating systems, solar cookers, and solar-thermal electricity generating
systems.

1. Introduction past few years. An ample number of approaches were scrutinized,

The evident paradox between the expanding energy demand, envi­
ronmental awareness, and dependency on fossil fuel has manifested a
continuous quest for alternative clean and renewable energy sources
[1]. Solar energy is one of the most abundant and inexhaustible sources
of green energy and has been probed as one of the primary fossil fuel
alternatives driving an immense amount of attention among the
research community in the past decade. PCM has been recognized as one
of the effective solar thermal energy harvesting schemes due to its
simplistic mechanism, high-energy conversion, and direct energy har­
vesting. Its ability to seamlessly charge and discharge an immense
magnitude of thermal energy during phase change transition without
any harmful emission magnified substantial interest [2].
Solar-mediated PCMs have acquired considerable attention in the
aiming for solar to heat energy conversion efficacy of PCMs. One of the
leading advancements toward PCM development is thermal conductiv­
ity modification, various conductivity supplements were implemented
such as CNT, GO, carbon black and various carbon resources [3–5].
Hence, these articulated thermal conductivity improvements are still not
enough to enunciate the basic constitution and mechanism of the
light-to-heat energy transformation [6,7]. Therefore, to fully cultivate
and harvest solar energy one should thoroughly consider the photo­
thermal transition mechanism. For effective solar to thermal energy
conversion, light absorption across the entire solar spectrum range and
potent light to heat conversion efficiency are of equal importance. Solar
absorption efficacy is one aspect of photo energy cultivation, the other
aspect is the effective conversion of these absorbed light photons into an
accessible form of energy [8] Broadband solar spectrum absorption and

* Corresponding author.
E-mail address: hernkim@mju.ac.kr (H. Kim).

https://doi.org/10.1016/j.solmat.2022.112075
Received 14 June 2022; Received in revised form 27 September 2022; Accepted 18 October 2022
Available online 1 November 2022
0927-0248/© 2022 Elsevier B.V. All rights reserved.
A.M. Pornea and H. Kim
techniques for effective photothermal conversion are essential for
attaining optimum solar energy harvestings [9]. Wang et al., prepared
an incorporated SiO2, CNT and PDA as a confining shell to insinuate
absorption spectra covering the entire solar spectrum for effective solar
energy harvesting [10]. Li et al., constructed a hierarchical zeolitic
imidazolate framework (ZIF) that was directly grown on carbon cloth,
The flexible scaffold infused with PCMs projected a broadband solar
absorption spanning the UV–Vis–NIR range for optimal spectral ab­
sorption [11]. Consecutively, strategies for the advancement and initi­
ation of effective photothermal conversion mechanisms are postulated
and can be categorized as; (1) electron-hole generation and relaxation
(2) localize plasmonic heating and (3) molecule thermal vibration [12,
13]. The revelation of the localized surface plasmonic resonance (LSPRs)
of doped semiconductor particles which were formerly assumed to be
distinct on metallic nanostructures only has introduced a new domain in
plasmonic engineering. Doping these nonmetallic nanostructures has
been proved to alter and equipped LSPR capability with escalation on
the hole carrier concentration supplementing redshift towards the NIR
range. This technique also articulated the limitation on the tunability in
the free charge carrier concentration of noble metals [14,15]. The LSPR
can highly manifest intense light absorption and photothermal conver­
sion potential promoting effective solar energy utilization. Tang et al.
published a PEG/Ti3C2Tx layered composite polyethylene glycol (PEG)
with extraordinary photothermal transformation and storage capability
which can be accounted for the innate nature of Ti3C2Tx, the composite
conveyed the LSPR effect which bestowed the composite PCMs with an
eminent photothermal conversion efficiency [16]. Likewise, a similar
group exhibited a complementary mechanism through the fabrication of
Ag-graphene/PEG composite, the generated material insinuated an
excellent energy conversion efficiency which can be ascribed to the
introduction of Ag particles that demonstrated LSPR due to its selective
absorbance in Vis-NIR [17].
Traditionally, distinct photothermal materials transform solar to
heat energy following a single mechanism. However, with the freedom
and flexibility to gratify utilization requirements by combining the
intrinsic properties of the constituting materials to enhance the light-
harvesting capability. More than one mechanism can be implemented
and postulated by combining these photothermal materials in an effec­
tive structural framework [2,18,19]. In this communication, we devise a
heterogeneous core-satellite assembly fabrication of a photoactive PCM
encapsulating shell constituting silica (DS), engineered plasmonic
nanoparticles (PG), and photosensitizer (PDA) for effective light to heat
energy harvesting and conferred as DS-PDA/PG. The conjugation of the
PCMs core and PG satellite to administer localized plasmonic heating
assisted by a PDA linker that enunciates molecule thermal vibration was
cited to be a practical approach to systematic photothermal energy
harvesting [20]. The rational design cultivated a wide solar spectrum
absorption and demonstrated effective dissipation of absorbed photon
energy through its corresponding structural motif. Due to its active
absorbance in the NIR range, PB serves in fields of application as a
photothermal conversion agent [21,22]. In this regard, we equipped PB
with LSPR through the introduction of Gd3+ ions onto the PB lattice
sites, and the generated nanoparticles were identified as PG. Interest­
ingly the introduction of Gd3+ ions onto the PB rendered a redshift of 30
nm which can also be ascribed to the LSPR property of PG. Hence,
despite the improved photothermal capacity, PG is still insufficient to
fully govern the entire solar spectra due to its limited intrinsic absorp­
tion activity at UV and early Vis ranges. To harness the entire solar
spectrum, PDA was utilized to address the absorption limitation of PG at
the visible light range and as an arresting media for PG. The presence of
PDA stimulates and accentuated absorption at the visible light range to
encompass the entire solar spectrum, PDA also promoted molecule
thermalization through its π-system which enhances the charge carrier
separation by channeling the photoexcited electrons to the interface
sites while dissipating heat once stabilized to ground state [2,23]. The
strategic union and structural arrangement of PG and PDA endowed
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Solar Energy Materials and Solar Cells 250 (2023) 112075
absorption on the entire optic gamut and advocated effective energy
conversion through localize plasmonic heating and molecule thermal
vibration, the distribution of the PG particles onto the shell interface
conversely dissipates the absorbed light photons as heat that leads to
improved localized heating. The presented material assimilation and
structural arrangement illustrated a significant prospect of direct photo
energy employment in diverse solar-mediated PCM applications such as
temperature management of greenhouses, solar water heating systems,
solar cookers, and solar-thermal electricity generating systems.
2. Experimental
2.1. Materials
n-Docosane (99%), tetraethyl orthosilicate (TEOS, 98%), formamide
(98%), hydrochloric acid (HCl, 36.5–38%), and Potassium hex­
acyanoferrate (III) (K3[Fe(CN)6], 98+%) were commercially obtained
from Alfa Aesar. Cetyltrimethylammonium bromide (CTAB) was
commercially supplied by Daejung Reagents Chemicals. Poly­
vinylpyrrolidone (PVP) and dopamine hydrochloride (DA) was pur­
chased from Sigma Aldrich. Gadolinium (III) nitrate hexahydrate (Gd
(NO3)3, 99.9%) was purchased from Acros Organics. All reagents were
used as received without further purification.
2.2. Preparation of PG nanoparticles
The Pb–Gd nanoparticles were fabricated through the traditional
hydrothermal synthesis route. First, a clear solution (Solution A) was
obtained by mixing 5 g PVP, 160 mg K3[Fe(CN)6], and 50 ml 0.01 M
HCl. Another solution was prepared by mixing 5 g PVP, 225 mg Gd
(NO3)3, and 50 ml 0.01 M HCl to acquire a clear solution (Solution B).
Subsequently, Solution A was slowly dropped to Solution B under
vigorous stirring for 3 h the solution was then transferred to a Teflon-
lined reactor and was placed in an electric oven for 24 h at 80 ◦ C. The
PG nanoparticle was centrifugated at 12,000 rpm for 30 min and washed
for three time followed by freeze drying process.
2.3. Synthesis of DS-PDA/PG capsules
Construction of DS-PDA/PG core-satellite through external confine­
ment of the PG nanoparticles onto the DS capsule interface assisted by
PDA. The interfacial modification was done by traditional conjugation
of PDA layer was prepared as previously reported [2], alongside with
this a distinct quantity of PG particles were introduced to the aqueous
suspension allowing PG to intercalate during PDA layer formation. For
comparative purposes, clean DS-PDA capsules were also prepared.
Alongside this, for the preparation of the DS-PG capsules, the same
procedure was followed for the synthesis of DS just an addition of a
certain amount of PG was introduced to the curing stage of the capsules.
Relative to the investigation of the effect of the structural arrangement
of the materials on the photothermal performance, DS-PG-PDA capsules
were prepared. The DS-PG capsules were then modified with a PDA layer
deposition. The core-satellite was prepared following the direct depo­
sition of PDA with the presence of PG nanoparticles. Different amounts
of PG particles were introduced onto the aqueous suspension,
DS-PDA/PG1, DS-PDA/PG2, and DS-PDA/PG3 for the PG amount of 25,
50, and 75 mg.
2.4. Characterization
Field emission scanning electron micrographs (FE-SEM) are
employed to illustrate the morphological features of the synthesized
capsules, while interfacial surface characteristics were revealed by
elemental mapping energy dispersive X-ray spectrometer (EDX, Hitachi
S–3500 N) at 5B to 92U. Fourier-transform infrared spectrum (FTIR,
Thermo Scientific Nicolet iS5) with a scanning range of 32 in the
A.M. Pornea and H. Kim Solar Energy Materials and Solar Cells 250 (2023) 112075

Fig. 1. (a) Schematic illustration of the synthesis technique of DS-PDA/PG capsules and its (b) relative photothermal conversion mechanism.

Fig. 2. SEM and EDX mapping of the fabricated capsules and their corresponding precursor (a,e) PG, (b,f) DS, (c,g) DS-PDA, and (d,h) DS-PG.

4000− 400 cm− 1 and resolution of 8 cm− 1 and X-ray photoelectron
spectroscopy (XPS, Thermo Electron) using Mg Kα radiation was
implemented to predict the functional groups of the generated capsules.
The optical characteristic of the generated capsules was tested through
Uv/Vis spectrophotometer (Thermo Scientific, Evolution 220). Struc­
tural features of the fabricated PCM were explored via X-ray diffraction
(XRD) using X’pert MPD diffract meter with a Bragg angle ranging from
5 to 90◦ to record the XRD patterns (Cu–K radiation = 1.540 Å). The
photothermal performance of the hybrid capsules was acquired using an
FTIR camera (COX, CX-Series). The photoelectrochemical examination
was scrutinized by taking the electrochemical impedance spectroscopy
(EIS) and linear sweep voltammetry (LSV) using an electrochemical plot

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A.M. Pornea and H. Kim
Fig. 3. SEM and EDX mapping of the fabricated capsules with various structural assembly and combinations (a,e) DS-PG-PDA, (b,f) DS-PDA/PG1, (c,g) DS-PDA/PG2,
and (d,h) DS-PDA/PG3.
set-up (SIVE SP1) with 1 M Na2SO4 utilized as an electrolyte at ambient
operating conditions. The electrodes were devised by drop-casting of 10
μL paste onto a 0.5 cm × 0.5 cm acid-treated carbon cloth. The paste
contains particles of DS-PDA/PG (2 mg) (or its corresponding counter­
parts) that were mixed with 50 μL DMF solvent and 10 μL Nafion binder.
The measurements were achieved with a traditional three-electrode set-
up, Tafel plots were measured with a scanning rate of 1 mV s− 1, and EIS
was assessed at OCP with 10− 2–105 Hz of the frequency gage. The sta­
bility of the materials was gauged by thermogravimetric analysis (TGA
N-100, Scinco) under an N2 atmosphere (50 mL min− 1), exposed at a
temperature ranging from 30 to 800 ◦ C with a ramping rate of 10 ◦ C
min− 1.
3. Results and discussion
3.1. Structural characterization of DS-PDA/PG capsules
Inspired by the apparent advantage of the structural architecture of
the PCM encapsulating shell on solar energy harvesting and storage
[24]. A core-satellite EPCM shell was strategically designed and oriented
as shown in Fig. 1a. The postulated arrangement entails the
core-satellite structure instigated by the PG nanoparticle deposition
assisted by PDA layer formation onto the pre-encapsulated DS capsules.
The intrinsic properties of the compounding materials were situated to
actuate wideband solar absorption covering UV, visible, and NIR light
spans, while their corresponding assembly facilitated effective light
harvesting and heat dissipation.
To illustrate the structural characteristics of the decorated capsules
and their corresponding counterparts, SEM imaging was performed as
showcased in Figs. 2 and 3. The design framework intends to cover
broad light absorption through compounding and effectively arranging
the photoactive materials onto the EPCM interface. The SiO2 encapsu­
lated PCM will serve as a base capsule for the structuralization of the
core-satellites. Following the previously presented approach, the shell
construction was facilitated by a conventional silica encapsulating
technique reinforced through an emulsifier. The distinct spherical ar­
chitecture of the DS capsules can be discerned as shown in Fig. 2b. The
generated DS capsules were then assimilated with PDA and PG to
augment solar activity. The PDA-coated capsules (DS-PDA) were
accomplished through conventional oxidative self-polymerization of
dopamine, and the formation of the PDA layer was revealed through
SEM imaging. It can be observed that the PDA incorporation managed to
maintain the spherical attributes of the capsules although an increase in
the surface roughness is perceived accounted to the successful formation
of the PDA layer as shown in Fig. 2c. On the other hand, the PG
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Solar Energy Materials and Solar Cells 250 (2023) 112075
nanoparticles instigated a cube-like structure like its PB predecessor
with a rounded corner which corresponds to the structural effect of the
Gd ions on its molecular structure as shown in Fig. 2a. A comparative
structural comparison of PB and PG were illustrated in Fig. 4 a-b.
Moreover, the PG-assisted capsules (DS-PG) were prepared through
electrostatic attraction, during the oil-water emulsion stabilization, the
SiO2 shell attributed a negatively charged interface enabling the arrest
of the positively charges PG nanoparticles. The affluent integration of
PG nanoparticles can be perceived in Fig. 2d, where robust amounts of
PG nanoparticles were pinned and incorporated onto the DS encapsu­
lating shell.
Along with different component alterations, structural framework
arrangements were also fabricated for comparative purposes elucidating
the advantage of the arrangement compounding material. The gener­
ated DS-PG capsules were then modified and deposited with the PDA
layer (DS-PG-PDA) to manifest the integral comparison of the materials
arrangement effect onto the light-thermal energy conversion relative to
the core-satellite. It can be recognized that the PDA layer deposition
instituted a smoother and finer interface covering the rough and intri­
cate framework of the deposited PG nanoparticles while still maintain­
ing its spherical characteristics as shown in Fig. 3a. Hence, the
morphological characteristics of the assembled DS-PDA/PG core-satel­
lites and their corresponding variations were presented in Fig. 3 b-d. The
PDA and PG incorporation were inspired by external confinement as­
sembly wherein a certain amount of the nanoparticles were present
along with the construction of the PDA layer, this allows the insertion of
the PG nanoparticle onto the crevice of the PDA structure. The intro­
duction of PDA along with PG nanoparticles instigated a subtle contri­
bution to the particle’s size while heightening surface roughness. A
series of trials involving various PG incorporating amounts were facili­
tated to consolidate its integration. It can be discerned that there is no
distinct morphological evolution in these varied PG incorporated sam­
ples, all demonstrating a spherical attribute. The increase in the PG
nanoparticle inclusion projected an evident increase in the particle size
and interfacial roughness, affirming the successful establishment of the
PDA and PG layer. The distinct core-satellite structural motif of the
generated DS-PDA/PG capsules was further investigated through TEM
imaging revealed in Fig. 4 c-e to elucidate its structural framework and
interfacial attributes. The apparent architectural arrangement of PDA
and PG onto the confining shell can be realized, and the direct assimi­
lation and arrest of PG onto PDA can be discerned. The illustrated
fabrication strategy signifies an excellent proficiency for direct incor­
poration of the component material.
A.M. Pornea and H. Kim
Fig. 4. TEM images of PB, PG (a–b) and DS-PDA/PG core-satellite (c–d). STEM-EDS line-scan profile (e) of the synthesized DS-PDA/PG capsules.
3.2. Optical and chemical characterization of DS-PDA/PG capsules
Excellent photothermal material is expected to be active on the
entire solar spectrum (Uv–Vis–NIR) to ensure effective solar energy
harvesting. Wideband solar spectral absorption is necessary for direct
light to heat conversion to harvest the optimal energy. The materials
absorption efficacy is one of the key parametric for effective solar energy
harvesting. The solar energy dissemination onto the earth interface
stretches a wide range from 100 nm to 2.5 μm which comprises the
following potion: the ultraviolet (Uv) band (100–400 nm, accord to the
~3% of the entire solar spectra), the visible (Vis) band (100–400 nm,
accord for the ~45% of the entire solar spectra), and the near-infrared
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Solar Energy Materials and Solar Cells 250 (2023) 112075
(NIR) band (700 nm-2.5 μm, accord to the ~52% of the entire solar
spectra).
Doping of the PB nanoparticles was performed to insinuate LSPR
property. A comparison of the spectral absorbance of PB and PG parti­
cles were presented in Fig. 5a. Both PB and PG demonstrated wide band
absorbance at ~700 nm, which can be ascribed to the metal-to-metal
charge transport between FeII and FeIII through the cyanide bridges
[25]. An increase in the NIR spectral absorption can be discerned
assisted by the Gd3+ ion introduction. A redshift phenomenon can be
recognized which can be correlated to the LSPR property of the PG
particles. The redshift can be correlated to the change in electron density
and orbital due to the presence of Gd ions in the cyanide lattice [25], the
A.M. Pornea and H. Kim Solar Energy Materials and Solar Cells 250 (2023) 112075

Fig. 5. Uv–vis (a–b) FTIR spectra (c–d), and XRD patterns (e) of the synthesized DS-PDA/PG capsules and their corresponding precursors and counterparts.

existence of the Gd3+ ion in the lattice disturbed the electron density and absorbance deviation.
orbital energies of the cyanide bonds which motivates the redshift of the To gauge the light-to-heat energy conversion and storage of the DS-
NIR spectral signature [26]. The Gd3+ ion engaged with the PB lattice PDA/PG capsules and their corresponding precursors, the light absorp­
site forming Fe–C–– N–Gd, reducing the [Fe(CN)6] vacancy. The decline
– tion characteristics of fabricated capsules and their relative assorted
in the presence of [Fe(CN)6] vacancy corresponds to the observed versions were investigated. The absorption signatures of the fabricated

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A.M. Pornea and H. Kim Solar Energy Materials and Solar Cells 250 (2023) 112075

Fig. 6. XPS patterns of the synthesized DS-PDA/PG capsules.

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A.M. Pornea and H. Kim Solar Energy Materials and Solar Cells 250 (2023) 112075

Fig. 7. Photothermal and photoelectrochemical features of the fabricated DS-PDA/PG and its respective counterparts. (a) photothermal chart, (b) temperature
difference under one solar irradiation relative to time, (c) ratio (R) of the temperature difference (ΔT) and incremented time interval (Δt), (d) temperature difference
under different solar sun irradiation, (e) cyclic photothermal chart, (f) FTIR camera images of the thermal propagation of the prepared capsules upon irradiation.

capsules were projected in Fig. 5b. Traditionally, silica-based material
projects an absorption performance at the Uv range as demonstrated by
DS capsules. On the other hand, the introduction of the PDA layer
revealed an increase in absorption intensity in the Uv and Vis range.
PDA resembles organic semiconductors due to its π-system which had
been effectively applied as a photosensitizer for the absorption of visible
light [2]. An absorption escalation can be realized upon the inclusion of
PG onto DS capsules, attaining absorption on the Uv and NIR with
minimal absorption on the Vis range resembling the PG nanoparticles,
with a slight intensity reduction. The DS-PG-PDA capsules on the other
hand projected a spectral absorption on the Uv–Vis with a scant activity
at the NIR range assimilating the intrinsic activity of the compounding
precursor. The reduction in the absorption at the NIR range can be
correlated with the formation of the PDA layer covering and reducing
the photon access of the PG particles. The core-satellites demonstrated
an effective integration of the precursor material attaining absorption
amplitude at the Uv–Vis–NIR range, demonstrating the structural motif
effectiveness. All core-satellites exhibit an analogous absorption per­
formance to their predecessor materials with an intensified absorbance
in correlation with the PG assimilation. The effective structural
arrangement equipped the EPCM with a wide solar spectrum absorption
fully utilizing the intrinsic properties of the precursor materials.
Conferred in Fig. 5 c and d are the FTIR spectra of capsules with
different shell components and structural arrangements. The band
associated with the symmetric and asymmetric stretching fluctuation of
Si–O–Si bonds was depicted at 800 cm− 1. The PDA layer deposited
samples maintain their precursor spectral peaks though a minimal in­
tensity reduction can be observed. For PG decorated samples, a distinct
peak located at 2075 cm − 1 was recognized which can be ascribed to the
presence of gadolinium hexacyanoferrate, manifesting the presence and

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A.M. Pornea and H. Kim
Fig. 8. (a–b) LSV and EIS profiles of the capsules with and without irradiation.
attachment of Gd3+ ions onto the cyanide bonds. This determines the
incorporation of the PG nanoparticles onto the encapsulating shell. A
peak progression comparison of the doped and undoped PB has also
been presented to illustrate the effect of the Gd ions incorporation onto
the PB lattice structure, a gradual shift at 2087 to 2075 cm− 1 can be
discerned which is associated with the covalent attachment of Gd ions
onto the cyanide bonds in the lattice [26]. While the bands located at
1630 and 3400 cm− 1 can be noticed across all samples, these bands can
be ascribed to the bending vibration of the O–H bond for the chem­
isorbed and free water, which is primarily influenced by the SiO2 hy­
drophilicity. Moreover, the spectra of the samples with varied PG
incorporation were presented in Fig. 5d and S1, a progressive increase in
the dominant peak can be noticed upon elevation on the PG amount
deposition.
Interpretation of the crystal structure of the prepared capsules was
actuated through XRD patterns projected in Fig. 5e. It can be realized
that all of the fabricated samples projected a complementary peak
analogous to that of pure n-docosane which was credited to its ortho­
rhombic crystalline planes corresponding to the standard JCPDS card
no. 45–1543 [24]. This implies that encapsulating shell does not affect
the crystallinity of the n-docosane ensuring effective reversible phase
change for thermal energy harvesting and storage. The diffraction peaks
located at 2θ = 17.48◦ , 24.75◦ , 35.00◦ , and 39.50◦ are linked to (100),
(110), (200), and (210) indexed to the traditional standard data cards of
PB JCPDS no. 01–0239. Moreover, the incorporation of Gd3+ ions
exhibited a (111) diffraction plane at 2θ = 15◦ associated with gado­
linium hexacyanoferrate, attributed to the covalent attachment of the
Gd3+ ions onto the cyanide bond lattice [26]. The incorporation of the
9
Solar Energy Materials and Solar Cells 250 (2023) 112075
PDA layer on the other hand did not project any apparent alteration and
appearance of new peaks, to the extent a gradual decrease in the peak
intensity of the PDA-covered materials might be recognized.
Elemental properties and distribution of the synthesized capsules
were thoroughly evaluated using SEM-EDX and TEM EDX projected in
Fig. 2 e-h and Fig. 3 e-h. The existence of Si and O elements in the
mapping report of DS capsules determines the successful formation of
the SiO2 shell. The PDA-coated DS capsules projected elemental traces of
C, O, and N affirming the establishment of the PDA layer onto the
encapsulating shell. For the DS-PG capsules, a clear demonstration of the
successful arrest of the PG particles is verified through the presence of C,
N, Fe, and Gd elemental signals. For the DS-PG-PDA, the absence of the
Fe, and Gd elemental profile compared to its precursor can be realized
which can be associated with the development of the PDA layer covering
the PG sites. Thereupon, for the DS-PDA/PG capsules, the presence of
the Fe and Gd spectra determines the successful assimilation of PDA and
PG onto the shell interface. In the case of the concomitant assorted PG
particle deposition, the mapping confirms the increase in the Fe and Gd
traces analogous to the PG incorporation amount. Moreover, an
elemental footprint reduction/elimination of Si and O can be distin­
guished in the subsequently treated samples instigated by the con­
struction of a layered shell. Furthermore, projected in Fig. 4e is the
STEM-EDS line-scan profile of the crafted DS-PDA/PG capsules, the line
scan affirms the elemental presence of Si, C, O, Fe, Ni, and Gd related to
the SEM-EDX mapping results with a heightened C signature attributed
to the presence of an immense amount of carbon-based materials.
The XPS testing was performed to further expound the elemental
attributes of DS-PDA/PG as projected in Fig. 6 a-e. The Si 2p scan profile
illustrated the binding energy located at 102.92 eV ascribed to the SiO2
confining shell, relatively, the O 1s spectra were also conferred. The C 1s
spectrum confirmed the presence of four peaks occupying the binding
energies 283.81, 284.72, 285.88 and 287.69 which can be associated
with C–C, C–N, and C–O bonds. The N 1s scan revealed the appearance
of two located at 396.78 and 399 eV. The Fe 2p spectra can be decon­
voluted into two peaks at 707.96 and 721.68 eV which were anointed to
the Fe2+ 2p3/2 and 2p1/2 [2,27]. The Gd 4d scan revealed two peaks
centered at 141.73 and 147.91 eV which can be ascribed to the Gd 4d5/2
and Gd 4d3/2 [28].
3.3. Photothermal and electrochemical performance of different shell
layer deposition and arrangement
Successful solar exhaustion can be obtained through the employment
of highly photoactive materials, due to good light attenuation and good
electron transferability PB and PDA had been mitigated in numerous
photothermal applications across field areas. PB has been utilized as a
photothermal agent, hence, the revelation of the localized surface
plasmonic resonance (LSPRs) of doped semiconductor particles has
introduced a new domain in plasmonic engineering. Therefore, we
engineered plasmonic nanoparticles by introducing Gd3+ ions into the
PB lattice structure, this facilitates the redshift of the NIR absorption
which confirms the LSPR property. Moreover, due to the limited ab­
sorption of PG in the visible light region, PDA was incorporated to
harness the entire solar spectrum. The highly photoactive shell was
insinuated through a direct assembly of PDA and PG nanoparticles onto
the DS shell, and effective light to heat energy conversion by adminis­
tering localized plasmonic heating and molecule thermal vibration.
Given the opportunity to manipulate the compounding materials and
structural integrity of the PCM encapsulating shell to augment the light-
harvesting capability insinuates the prospect to provide functional at­
tributes. The assimilation of the intrinsic attributes of the constituting
materials and their corresponding structural motif opted for a refined
strategy for photo energy cultivation. The photothermal response and
efficacy of the fabricated capsules were determined with the aid of a
solar simulator as presented in Fig. 12a. A scarce thermal shift can be
realized on DS samples as projected in Fig. 7 a-d, which can be
A.M. Pornea and H. Kim Solar Energy Materials and Solar Cells 250 (2023) 112075

Fig. 9. Photothermal and photoelectrochemical features of the fabricated DS-PDA/PG with varied PG incorporation. (a) photothermal chart, (b) temperature dif­
ference under one solar irradiation with respect to time, (c) ratio (R) of the temperature difference (ΔT) and incremented time interval (Δt), (d) temperature dif­
ference under different solar sun irradiation, (e) cyclic photothermal chart, (f) FTIR camera images of the thermal propagation of the prepared capsules upon
irradiation.

correlated to the limitation of the SiO2 to absorb photons. The PDA-
assisted capsule on the other hand prompted an instantaneous thermal
escalation ascribed to its ability to acquire light photons in the visible
range. Relatively, PG-enforced capsules demonstrated the same heating
profile with a moderate increase in thermal change. The imminent
thermal elevation can be associated with the activity of PG in UV and
NIR which corresponds to a higher light portion cultivation. Further­
more, a PDA layer was deposited on the DS-PG capsules interface, and an
incremental increase in thermal escalation can be discerned. On the
other hand, capsules in adverse structural motifs were facilitated, and a
heterogeneous core-satellite assembly was devised by conjugation of the
PCMs core and PG satellite assisted by a PDA linker [29]. A remarkable
thermal increase can be realized on the thermal profile of DS-PDA/PG
attaining a thermal elevation of 32.25 ± 1.43 ◦ C which is in sharp
contrast with DS-PG-PDA that only attained a thermal increase of 26.76
± 0.46 ◦ C even if it has the same constituting material. To further
expound on the discrepancy in the thermal difference of the prepared
capsules, the ratio (R) of the thermal change (ΔT) relative to the time
interval (Δt) is theorized and displayed in Fig. 7c. It can be perceived
that the incorporation of photoactive materials relatively illustrates a

10
A.M. Pornea and H. Kim
Fig. 10. (a–b) LSV and EIS profiles of the capsules with and without
irradiation.
propagated response relative to the constituting materials. The photo­
thermal influence of different solar power intensities (0.5, 1, 1.5, and 2
W cm− 2) was also thoroughly scrutinized and presented in Fig. 7d. As
anticipated DS-PDA/PG manifests the highest thermal difference in all
the solar power settings. This concludes the impact of the rational
arrangement of PG and PDA on the effectiveness of solar energy culti­
vation. The design is intended to cover broad light absorption and
effectively cultivate these absorbed photons through compounding
photoactive materials and competent dissipation of absorbed energy. In
this case, DS-PG-PDA can not properly mitigate the full capacity of the
incorporated materials since the PDA hampers the photons absorbance
on the PG sublayer. As per DS-PDA/PG, where both photoactive mate­
rials are equally exposed to light irradiation which constitutes broad­
band spectral absorption and exploitation of the LSPR property of the
engineered PG nanoparticles. To articulate the recyclability of the
DS-PDA/PG capsules, cyclic irradiation was facilitated for 700 s heating
followed by 700 s cooling as shown in Fig. 7e. The repetitive heating and
cooling affirmed the light to thermal stability performance of the com­
posite shell achieving the same thermal peak in every cycle.
To elucidate the solar irradiation response of the generated capsules,
LSV measurement was performed. The samples were secured on a piece
of carbon cloth electrode as mentioned in the experimental section. The
LSV assessment was measured within − 1− 0 V potential range by
applying a 1 mV s− 1 scan rate under dark and irradiated conditions as
presented in Fig. 8a. It can be realized that all the samples demonstrated
an elevated photocurrent upon irradiation which corresponds to the
ability of the constituting materials to accept light photons. Hence, DS-
11
Solar Energy Materials and Solar Cells 250 (2023) 112075
PDA/PG2 demonstrated the highest photoexcitation efficacy. Moreover,
EIS measurements were facilitated and presented in Fig. 8b to verify the
electrochemical performance of the articulated capsules. All the Nyquist
profile demonstrates a conventional impedance arc with an ascending
trajectory. DS-PDA/PG2 demonstrated the least impedance curve which
corresponds to its effective structural framework that dissipates elec­
trons seamlessly throughout the encapsulating shell followed by DS-PG-
PDA, DS-PG and DS-PDA.
3.4. Photothermal and electrochemical performance of different PG
particles incorporation
Once the PG and PDA assimilation and structuralization in a core-
satellite manner were confirmed, a variation on the incorporated PG
was construed since it gravely influences the photothermal efficacy of
the designed capsules, the PG incremental amounts were listed in
Table S1. The photothermal characteristics of the EPCM with different
PG content were investigated. Its corresponding thermal progression
were presented in Fig. 9(a–e). All of the DS-PDA/PG capsules achieved
an identical heating profile but with different optimal temperatures. The
DS-PDA/PG3 rendered the thermal shift reach up to 64.50 ◦ C with a
thermal change of 33.22 ± 1.39 ◦ C. Which was followed by DS-PDA/
PG2 obtaining an optimal temperature of 62.15 ◦ C with a thermal dif­
ference of 32.25 ± 1.43 ◦ C, and DS-PDA/PG1 acquiring a maximum
temperature of 58.40 ◦ C with a thermal increment of 28.89 ± 1.21 ◦ C.
This confirms the PG nanoparticles effect on the photothermal efficacy
of the EPCM, demonstrating that the quantity of the incorporated PG
nanoparticles is analogous to the temperature change. Upon examina­
tion of the R-value, as projected in Fig. 9c, it is realized that the increase
in thermal change is highly influenced by the incorporation of PG
nanoparticles, identifying DS-PDA/PG3 with the highest thermal change
which can be associated with its higher activity on NIR spectral range
[12]. Furthermore, an apparent temperature elevation can be realized
upon the increase in light irradiation as illustrated in Fig. 9d.
The illumination excitation of the DS-PDA/PG and its corresponding
counterparts were also determined through LSV and EIS measurements
as shown in Fig. 10 a-b applying the previously mention parametric
condition. All the measured samples demonstrated an improved LSV
curve which corresponds to the illumination activity. Analogously, the
rendered photocurrent follows the trend of incorporating PG nano­
particles. A considerable incremental change in the current with respect
to the potential of the PG decorated capsules can be discerned. The DS-
PDA/PG3 administered the optimal electrochemical response which can
be attributed to its plasmonic ability. Relatively, the EIS data follows the
same trend as shown in Fig. 10a. All Nyquist curves follow the same
trajectory, with DS-PDA/PG3 demonstrating a higher angular path,
followed by DS-PDA/PG2 and DS-PDA/PG1 respectively.
3.5. Phase change and thermal energy performance of DS-PDA/PG
microcapsules
The thermal durability of the confining shell of the PCM is critical
due to subsequent exposure to high and low temperatures. The thermal
characteristics of the fabricated DS-PDA/PG capsules and their corre­
sponding counterparts were measured using TGA analysis as illustrated
in Fig. 11a. All of the representative samples projected a one-step
thermal deterioration. The structural attributes of fabricated capsules
through its thermal degradation progression, the pristine n-docosane
was fully degraded upon reaching the temperature of 243.24 ◦ C sug­
gesting its pure hydrocarbon constitution. On the other hand, upon
confinement with a SiO2, an apparent improvement in the stability can
be realized with a residual amount of 18.70%. The introduction of the
PDA layer constituted a slight stability improvement which can be ar­
ticulated in its polymeric property. Moreover, the incorporation of PG
particles onto the DS capsules followed the same degradation profile as
the PDA-assisted capsules. A hefty shift in the decay profile can be
A.M. Pornea and H. Kim
Fig. 11. Illustrations of (a) Thermal attributes investigation and (b–d) DSC diagrams of the encapsulated pure n-docosane and its corresponding subsequent
encapsulated particles.
discerned upon the subsequent interlayer deposition of SiO2, PG and
PDA onto the confined PCM. Moreover, simultaneous assimilation of
PDA and PG onto the encapsulated PCM projected enhanced thermal
stability, which can be ascribed to its better association with the
incorporating materials and the PCM capsules. An improvement can also
be realized on the incremental increase in the amount of residue of core-
satellites. The observed stability enhancement can be attributed to the
intrinsic property of PG nanoparticles. The integration of PDA and PG
augments the stability characteristic of the confined PCM with a definite
decrease in the weight ratio of the n-docosane. It is anticipated that the
amplified deposition volume thus forms a protective layer inhibiting the
abolition of the fabricated capsules. This realization can be correlated to
the ability of the confining shell to avert leakage and degradation of the
docosane core. Furthermore, the generated capsules attained an ample
amount of char residue (>20%), in which the char yields proportionally
relate to the mass fraction of the docosane relative to the confining
material.
The phase transition characteristics of the fabricated capsules were
examined through DSC, and the relative heating and cooling profiles,
temperature change and enthalpies were shown in Fig. 11b–d. All pro­
cessed samples projected a dual endothermic spike commending phase
transition progression of the docosane due to the solid-solid and solid-
liquid conversion, this can be ascribed to the phase alteration from an
ordered state to a disordered state upon DSC testing. Assuming that
there is no chemical reaction between the PCM and the confining shell,
the assembled capsules observed an identical melting and crystallization
trajectory. The melting temperature (Tm) and crystallization tempera­
ture (Tc), melting enthalpy (ΔHm), and freezing enthalpy (ΔHc) for
12
Solar Energy Materials and Solar Cells 250 (2023) 112075
pristine docosane 41.00 ◦ C and 33.00 ◦ C, 248.00 J/g and 248.00 J/g.
The evident crystallinity of the docosane is distorted by the heteroge­
neous nucleation effect of the capturing shell onto the Tc and Tm of the
assembled capsules. Hence, there’s a minimal discrepancy in Tc and Tm
upon the addition of PDA and PG. However, all the confined samples
posted a reduced ΔHm and ΔHc due to the incremental portion eleva­
tion of the confining shell. The constraint relative to the phase change
enthalpy of docosane is shown in Table S1, following the fractional in­
crease of the encapsulating shell which severely reduced the specific
enthalpic capacity of the EPCM. To demonstrate the recyclability of the
designed core-satellite EPCM, repetitive thermal cycles were performed.
The subsequent thermograms were demonstrated in Fig. S2 a and b,
surprisingly, the DSC profiles still overlap after undergoing repeated
heating and cooling conveying almost the same chart. This signifies that
the generated DS-PDA-PG capsules have vast phase-transition profi­
ciency to retain thermal successive energy storage and release. The
structural characteristics of the thermally cycled capsules were exam­
ined through SEM imaging as shown in Fig. S2 c and d, the core-satellite
shell layer exhibited significant stability upon exposure to recurrent
heating and cooling. This can be recognized in the enthralling articu­
lation of the joint synergy of the compounding materials in an arranged
manner, suggesting that the configuration of the SiO2, PDA and PG
administers an excellent conservation ability of the capsuled PCM
ensuring mechanical plasticity to endure repetitive heating and cooling.
It can be determined that the coherent EPCM in this communication has
beneficial thermal effectiveness and structural dependability for effi­
cient and effective solar-thermal energy harvesting.
A.M. Pornea and H. Kim Solar Energy Materials and Solar Cells 250 (2023) 112075

Fig. 12. (a) Experimental setup for illumination photothermal investigation and (b) DS-PDA/PG photothermal mechanism.

3.6. Light to the thermal conversion efficiency and mechanism photo energy harvesting which is highly influenced by the ability to
harness immense magnitude of light to convert it into an accessible
mode of energy. The improved light-to-heat transformation of the
m ΔHm
η= ( ) Eq (1) generated DS-PDA/PG capsules through broadband light absorption and
AP tfinal − tinitial enhanced solar-to-heat transformation was thoroughly investigated. The
Solar to thermal conversion efficacy is one of the most vital facets of solar to thermal transformation ability of the fabricated capsules was

13
A.M. Pornea and H. Kim
affirmed using Equation (1), where η stands for the light to thermal
energy conversion efficiency, ΔH is the melting enthalpy of the sample,
m is the sample weight, A is the illuminated area, P is the power density
of the light used and tfinal and tinitial is the initial and final time of the
melting process [7,10]. As presented in Figs. 12a, 7a and 8a, a pro­
gressive thermal increase can be realized upon illumination, these fig­
ures are recapitulated to accentuate the phase transition of the confined
PCM. Projected in Fig. 12 c-d, is the magnified temperature progression
exhibiting the phase transformation of the encapsulated docosane, the
altered temperature attenuation was marked by defining the junction
where the melting phase occurs. From these, the respective conversion
efficiencies are derived using equation (1). It can be realized that even
though DS-PDA/PG3 attained the highest thermal increment and the
fastest melting transition, the elevation on the fraction of the confining
shell imposed an eradication on the conversion efficiency. The fractional
elevation of the confining shell directly influences the enthalpic capacity
of the EPCM to absorb and release thermal energy as observed in the
TGA and DSC data. Considering the energy storage and release insinu­
ation, it can be concluded that DS-PDA/PG1 is the preferred encapsu­
lation condition to attune the energy capacity of the EPCM while
maintaining its photothermal performance. It should also be noted the
thermal elevation and the melting phase transition is minimal since the
PG-assisted capsules follow the same thermal profiles.
To further enunciate the photo energy accumulation ascribed to the
improved solar energy cultivation through wide band solar absorption
and efficient photothermal energy conversion by the assimilation of PG
nanoparticles to administer LSPR and PDA linker that enunciates
molecule thermal vibration. The structural arrangement enunciates an
improvement in the effective dissipation of absorbed photon energy. As
projected earlier the core-shell satellite structural motif demonstrated
superior performance compared with its corresponding counterparts.
Moreover, the core-satellite approach impacts the photothermal per­
formance through the strategic positioning of the PG-actuated particles
onto the encapsulating shell interface [19,30,31]. This structural strat­
egy leads to a direct synergy between the compounding materials that
constitute and augment the performance by initiating seamless inter­
action within the structured shell dissipating heat effectively. As pro­
jected in Fig. 12b, the intrinsic property of the compounded materials
articulated specific contributions to photothermal conversion. The sys­
tematic material arrangement constituted the coupling manifestation,
the close proximity of the PG nanoparticles allows their plasmons to be
coupled ensuing in an effective electron distribution [32]. Moreover, the
strong interaction coupling between the PG and PDA within the
encapsulating shell construed a pathway for seamless electron move­
ment throughout the structured confining shell for effective thermal
distribution [33].
4. Conclusions
In the conferred communication, an exceptionally effective light to
thermal energy conversion approach is systemized through a simplistic
fabrication technique of a photoactive PCM encapsulating shell consti­
tuting silica, engineered plasmonic nanoparticles (PG), and photosen­
sitizer (PDA) for effective light to heat energy harvesting was presented
(DS-PDA/PG). The developed heterogeneous core-satellite through
linking the PCMs core and PG satellite to promote LSPR heating sup­
ported by a PDA linker that articulates molecule thermal vibration. The
illustrated technique presented an innovative insight for effective
cultivation of solar energy ensuring that a substantial percentage of the
energy absorbed transforms to heat effectively. The curated approach
achieved a phase transition enthalpy of 139.20 J/g, with a thermal
discrepancy of 28.89 ± 1.21 ◦ C attaining an augmented photo to heat
energy conversion efficiency of 96.95% due to wideband solar absorp­
tion (UV–Vis–NIR) and effective heat dissipation through the core-
satellite assembly. The implemented approach in this study gathered
an appreciated contribution to PCM’s straightforward solar-thermal
14
Solar Energy Materials and Solar Cells 250 (2023) 112075
cultivation applications which can simply transmute to accommodate
several applications such as; temperature management of greenhouses,
solar water heating systems, solar cookers, and solar-thermal electricity
generating systems.
CRediT authorship contribution statement
Arni M. Pornea: Writing – review & editing, Writing – original draft,
Visualization, Validation, Methodology, Formal analysis, Data curation,
Conceptualization. Hern Kim: Writing – review & editing, Resources,
Project administration, Funding acquisition.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
The data that has been used is confidential.
Acknowledgment
This study was supported by Basic Science Research Program
through the National Research Foundation (NRF) funded by the Ministry
of Education (2020R1A6A1A03038817) and the Ministry of Science and
ICT (MSIT) (2020R1A2C2101759; 2020K1A3A1A30103645), Republic
of Korea.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.solmat.2022.112075.
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