Solar Energy Materials & Solar Cells 210 (2020) 110489

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Solar Energy Materials and Solar Cells

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

Plant-derived carbon nanospheres for high efficiency solar-driven steam

generation and seawater desalination at low solar intensities
Higgins M. Wilson, Tushar, Shakeelur Raheman Ar, Neetu Jha *
Department of Physics, Institute of Chemical Technology Mumbai, N.P. Marg, 400019, Mumbai, India

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

Keywords: In recent times, solar steam generation has proven to be an efficient method for seawater desalination. Herein,
Solar thermal we report a novel solar evaporator designed with plant-derived carbon nanospheres obtained from Cinnamomum
Camphor camphora incorporated in a polyvinyl alcohol sponge (C@CPVA). The fabricated evaporation device produced
Interfacial evaporation
steam at a rate of 1.53 kg m 2 h 1 under 1 sun illumination which was 3.25 times the bare water system. The
Desalination
Carbon nanospheres
device further exhibited an outstanding photothermal efficiency of 92.38%, owing to its indirect capillary water
pathway design. Furthermore, the C@CPVA array, when integrated in a facile laboratory solar still, generated
clean water with an excellent salt removal efficiency of 99.99%. The C@CPVA solar still had exceptional per­
formance even at low, non-concentrated solar intensities, thus enabling its application in practical solar desa­
lination. Finally, the distinct merits of C@CPVA solar still such as excellent low solar intensity performance,
facile fabrication and low cost advocate its rapid scaling up to large scale desalination systems. This work should
inspire further development of photothermal membrane-incorporated solar stills for non-concentrated, low-in­
tensity solar desalination.

1. Introduction generation by Halas group with the help of SiO2–Au nanoparticles

In recent times, solar-driven steam generation has piqued the interest
of those among the scientific community as a long-term solution for
water purification and water desalination [1,2].However, large-scale
applications have not come into fruition, owing to the concerns
regarding the inefficiency of sunlight absorption by water [3]. Water
primarily absorbs wavelengths in the infrared spectrum and displays low
absorption in the visible and ultra violet spectra. This is a major hurdle,
since the solar spectrum ranges from ultraviolet to infrared, with high
intensities in the visible range. This issue was initially addressed with
photothermal coatings designed to absorb incoming solar radiation [4].
The coatings, though beneficial in absorbing over a wider range of the
solar spectrum, lacked in overall efficiency and failed to produce con­
stant steam. Moreover, in most cases the intensity of solar illumination
was not optimal for water evaporation and required complex solar
concentrators to produce constant steam [4]. The discovery of plas­
monic nanoparticles and their high efficacy in photothermal heating was
a major breakthrough in the past decade. Plasmonic nanoparticles such
as gold and silver were found to produce heat by surface plasmon
resonance [5]. This phenomenon was then innovated for steam
tailored to absorb sunlight illuminations [6]. The nanoparticles were
dispersed in water and irradiated by sunlight to produce steam. The
nanoparticle dispersion showed a considerable increase in photothermal
efficiency and produced constant steam. Following that, various nano­
particles have been reported with similar approach for steam production
[7–10].
Even though nanoparticle dispersions were successful in improving
the efficiency of steam generation, they had disadvantages like
cumbersome recovery of nanoparticles, mediocre photothermal effi­
ciencies and so forth. These issues were first addressed by Ghasemi et al.
in their floating substrate-based solar-driven steam generation system,
where interfacial evaporation was facilitated using a floating substrate
[11]. The floating substrate had broadband absorbance which absorbed
incoming solar illumination. The absorbed light was then converted into
heat to create a localized heat zone at the surface. The porous substrate
enabled contact between the water molecules and the hot zone. The
water molecules evaporated spontaneously at the heat zone and
generated steam. The low thermal conductivity of the porous substrate
helped in maintaining the heat zone at the surface for constant steam
generation and the porosity of the substrate aided in the capillary action

* Corresponding author.
E-mail address: nr.jha@ictmumbai.edu.in (N. Jha).

https://doi.org/10.1016/j.solmat.2020.110489
Received 1 October 2019; Received in revised form 6 February 2020; Accepted 1 March 2020
Available online 5 March 2020
0927-0248/© 2020 Published by Elsevier B.V.
H.M. Wilson et al.
of water. Hence, the combined effects of broadband absorbance,
porosity, and low thermal conductivity resulted in a high photothermal
efficiency and facilitated constant steam generation. Various evapora­
tion devices based on floating substrates have been reported in recent
years [1,11–28]. A wide range of materials have been proposed for this
application, ranging from carbonaceous substances like carbon,
graphite, graphene oxide, and soot; inorganic materials like MoS2,
Mxene and polymeric materials such as aromatic cross linked polymers,
3D monolithic polypyrrole and so forth with excellent photothermal
efficiencies [26,29–36]. In this regard, Ito et al. designed a photothermal
membrane utilizing porous graphene as absorber material and obtained
a photothermal efficiency of 80% under 1 sun illumination [19].
Meanwhile, Li et al. developed a 3D printed carbon nanotube, graphene
oxide and nanofibrillated cellulose all in one evaporator with 85.6%
photothermal efficiency [20]. Li et al. demonstrated a jellyfish like
structure composed of carbon black, Graphene oxide and polysterene
foam matrix to obtain 87.5% 1 sun efficiency [22]. Furthermore, our
group recently demonstrated carbon fabric and diesel soot-cotton cloth
as photothermal membranes with 60% and 91.7% photothermal effi­
ciencies under 1 sun illumination [31,33]. Meanwhile, plant or biomass
based materials have also been reported as photothermal evaporation
devices such as carbonized mushrooms, carbonized daikon and so forth
with excellent photothermal efficiencies [26,37,38].
Currently the applicability of solar evaporators on a pragmatic scale
are limited due to some factors such as the cost of production of devices
in large scale systems, complexity of synthesis of photothermal materials
in bulk and toxicity of the materials. With an effort to overcome the
above limitations, we report a highly efficient, scalable and low-cost
photothermal evaporation device fabricated using carbon nanospheres
derived from camphor - a waxy transparent solid obtained from the tree,
Cinnamomum Camphora [39]. Camphor, a low cost, non-toxic and
abundant material is well documented for its medicinal applications in
Asia and Europe [39,40]. Camphor has a terpeniod structure (C10H16O)
with three methyl groups (CH3) and one carboxyl group (C– – O). On
partial or complete combustion of camphor, the methyl groups are
removed from the camphor ring to produce a highly reactive pentagonal
or hexagonal camphor skeleton structures [40]. The carbon nano­
particles obtained from the combustion of camphor are also reported to
be biocompatible, chemical inert and non-toxic [40]. In present work, a
facile thermolytic reaction of camphor wax was followed to produce
carbon nanospheres successfully with an average size of 50 nm. The
carbon nanoparticles were incorporated into polyvinyl alcohol sponges,
another low cost abundant material to obtain a novel solar-driven
evaporation device, which recorded a photothermal efficiency of
92.38% under 1 sun illumination. This is among the highest solar-driven
evaporation device efficiencies reported until now. The work also
focusses on the importance of indirect water paths for excellent thermal
management at the air-water interface, promoting interfacial evapora­
tion of water. Lastly, the evaporation device was extensively tested for
water desalination, and exhibited nearly 99.9% salt removal efficiency
even at low solar intensities.
2. Materials and methods
2.1. Materials
Camphor pellets (Cinnamomum camphora), polyvinyl sponge (PVA
sponge), polystyrene foam, and cotton cloth (100% pure) were procured
from a local grocery store. Ethanol (>98%) was obtained from Sigma
Aldrich, India.
Synthesis of plant-derived carbon nanospheres and carbon
nanosphere-coated PVA sponge (CPVA).
Synthesis of carbon nanospheres from camphor: Plant-derived carbon
nanospheres (CS) were synthesized by burning camphor pellets. While
the pellets were burning, a copper plate was placed at the top to collect
the black-colored soot. The copper plate was then allowed to cool, and
2
Solar Energy Materials and Solar Cells 210 (2020) 110489
the carbon nanoparticles were removed from the surface using a spatula
and stored for further usage.
Fabrication of CPVA: CPVA was fabricated by coating CS on PVA
sponge. PVA sponges were first cut into small discs of 4 cm diameter.
The thicknesses of the PVA sponges varied as 3 cm and 1 cm for com­
parison studies. The PVA sponges were later washed repeatedly in DI
water and dried at room temperature. In the next step, a CS solution was
prepared with carbon nanospheres and ethanol. The concentration of
the CS-ethanol solution was estimated to be 3 mg/mL. In the final step,
the top portions of the dried sponges were coated with the CS-ethanol
solution. The coated sponges were dried at room temperature and
recoated until the sponge surfaces were completely black. The coated
sponges were washed with DI water to remove excess particles and dried
for experimentation.
Fabrication of C@PVA and C@CPVA: The fabrication of C@PVA and
C@CPVA involved two steps. The first step was the synthesis of the
capillary-based indirect water path system. The capillary system was
designed using a polystyrene foam and cotton cloth setup. Polystyrene
foam discs of diameter 4 cm and thickness 3.5 cm were cut for this
purpose. In the cut pieces, horizontal silts of length 3 cm were made
horizontally at the top area. Moreover, a small window of 2 cm � 2 cm
was also created. Cotton cloth was passed through the horizontally cut
slits and allowed to fall towards ground from both sides. The C@PVA
and C@CPVA were finally assembled by cutting 2 cm � 2 cm pieces from
the PVA and CPVA sponges respectively and placed in the window
created in polystyrene foam and cotton cloth setup.
2.2. Characterization
The surface morphologies of CS, PVA, and coated PVA were analyzed
using Field Emission Scanning Electron Microscopy (FESEM, JSM-
7600F). Transmission Electron Microscopy (TEM, Tecnai G2, F30) was
used for high-resolution surface morphological studies. X-ray diffraction
pattern of CS was obtained using an X-Ray Diffractometer (XRD, Bruker
D8, Advance). The range of analysis was 10̊–80̊ with CuKα radiation of
wavelength 1.54 Å. The structure of CS was further studied using Raman
spectroscopy (Brukin RFS). Meanwhile, X-ray photoelectron spectros­
copy (XPS, PHI 5000 VersaProbe III) was utilized to study the compo­
sition of CS. Finally, the optical characterization of PVA and the coated
PVA sponges was done using Ultraviolet–visible spectroscopy
(UV–Vis–NIR, Perkin lambda 950).
2.3. Water evaporation performance evaluation setup
Water evaporation was analyzed using a solar simulator (Newport,
AAA, 94023A). A 100 mL borosil beaker was filled with DI water, and
the constructed evaporation systems were kept above the water. In the
case of C@CPVA and C@PVA evaporation systems, the water level was
less than 20 mL. The evaporation performance of both the systems was
examined for a period of 7200 s. The change in mass loss was noted at
intervals of 900 s using a digital weighing balance (Mettler, AE240). The
humidity and room temperature were maintained at 60% and 27 � C,
respectively throughout the experimentation. Dark evaporation rates
were measured by maintaining the earlier set-up, while covering the
entire system with a black box to completely block out light. Infrared
images were captured using a FLIR-ONE thermal camera module with an
accuracy of ~1̊ C. The bulk water temperatures and vapor temperatures
were measured using k-type thermocouples.
2.4. Water desalination study
Water desalination studies were conducted using a facile prototype
designed in the laboratory (Fig. S1). A cuboidal plastic box of size 20 cm
� 11 cm x 10 cm was procured from the local grocery store. The box was
then sectioned into two for seawater (obtained from the Arabian Sea)
storage and condensed water collection. Following this, the box was
H.M. Wilson et al.
modified into a trapezoid with top and bottom thicknesses of 8 and 3.5
cm, respectively. The top of the trapezoidal box was covered with glass,
with the aid of polystyrene foam for support. The glass window was
designed such that it completely covered the box with no leakage.
C@PVA systems with dimensions of 4 cm � 4 cm were arrayed to cover
the entire sea water section of the system. Water evaporation testing was
done by keeping the desalination setup under solar simulator with
varying intensities (0.5-1sun) for 2 h without any external disturbance,
at the end of which the condensed water was collected and weighed for
comparison with the bare sea water system. Finally, the desalination
performance was tested under natural sunlight for 6 h during the day.
For testing desalination prowess over a wide range of weather param­
eters, the setup was tested on days with varying weather conditions like
sunny and cloudy from 10 a.m. to 4 pm at humidity levels ranging from
70 to 80% in Mumbai, India. The condensed water was collected and
tested for its salinity using a pH-EC-TDS meter (Esico model 1615).
3. Results and discussion
3.1. Material design
In solar driven steam generation, scalability of the system for large-
scale application is vital. This can be achieved effortlessly if the solar
steam generator has a facile fabrication technique and can be assembled
with materials that are available in abundance. Additionally, a low
overall cost of fabrication is highly desirable. Hence, considering all
these factors, materials which are commonly available materials were
chosen to develop these evaporation devices. As shown in Fig. 1, floating
substrates were constructed with CS and PVA sponge. In the first step, CS
was obtained by burning camphor in air. The visible yellow flame
Fig. 1. Synthesis of carbon nanospheres (CS) from camphor and fabrication of
CPVA for solar steam generation.
3
Solar Energy Materials and Solar Cells 210 (2020) 110489
indicates incomplete combustion and soot generation by thermal
decomposition [41]. In our study, an average of 0.0138 g of CS was
collected from a single camphor pellet of mass 0.27 g. The obtained CS
was black in color, which suggested the possibility of broadband light
absorption. It should be noted that CS is also nontoxic in nature
compared to other reported hazardous soot particles such as diesel soot
[39].
CS was first visualized using SEM (Fig. 2a). The SEM images show an
agglomeration of carbon nanospheres. Upon further evaluation, the
particles seem to form a chain-like morphology with each spherical
particle attached to the other. This could be due to weak van der Waals
attraction between the particles. The particle distribution was further
examined using TEM (Fig. 2b). The TEM images confirm the chain-like
morphology of carbon spheres. The particle size was estimated to be
approximately 50 nm in diameter. Interestingly, the morphology of CS
was found to be similar to soot particles reported in literature [32,33].
Fig. 2b (inset) shows the Selected Area Electron Diffraction (SAED)
pattern of CS. The pattern exhibits the amorphous structure of CS. Poor
crystallinity of camphor soot was also noticed in the XRD pattern as
shown in Fig. 2c. Two broad peaks were observed at 24.9� and 43.6� ,
which can be assigned to the (002) and (111) lattice planes, respectively
[39].The (002) and (111) planes are associated with amorphous carbon
and diamond-like carbon materials, respectively [41]. The interlayer
spacing (d002) was calculated to be 3.58 Å. This value is analogous to
those of graphite layers in previous literature [42]. Raman spectroscopy
was used to study the structural defects of the carbon nanoparticles.
Fig. 2d displays the first order Raman spectra of CS. The spectra can be
characterized by the two bands at 1304 cm 1 (D band) and 1595 cm 1
(G band) [40]. The G band can be assigned to the crystalline graphite
structure which shows highly oriented pyrolytic carbon (sp2 hybridi­
zation). The D band stipulates the disorder in carbon indicating amor­
phous structure and presence of defects in the carbon structure. The
Raman spectroscopy data was further fitted using five bands, namely D1,
D2, D3, D4 and G [40]. The D1 band at 1304 cm 1 and D2 band at 1551
cm 1 represent the A1g symmetry mode and the E2g stretching mode,
respectively, the of disordered graphitic lattice located on graphene
surface. The D3 band (1483 cm 1) originates due to the presence of
amorphous carbon. Meanwhile, the D4 band could be due to the
stretching of C–– O and C– – C bonds. The ID/IG ratio of CS was calculated
to be 1.15, thus indicating the presence of defects in the structure. The
chemical composition of CS was further evaluated by XPS. As shown in
Fig. 2e, CS is highly carbonaceous with 95.53% carbon and 4.47% ox­
ygen content. Fig. 2f depicts the C1s spectra of CS. The C1s peak can be
deconvoluted into three peaks at 284.7 eV, 285.5 eV and 288.5 eV.
These peaks can be assigned to C– – C graphitic carbon peak (sp2 hy­
bridization), C–O hydroxyl peak and C– – O carboxyl peak respectively
(sp3 hybridization), respectively [31]. Finally, Fig. S2 shows the contact
angle measurement of CS. CS is hydrophobic with a contact angle
measurement of 125̊.
The next step in the design of the evaporation device is the selection
of substrate. An apt substrate in this aspect would be one which is
extremely hydrophilic for constant supply of water; is flexible and robust
for repeated usage; has low thermal conductivity (0.3 W m 1K 1) for
heat localization; and porous for capillary action of water (Fig. S3). One
such substrate that meets all the above requirements is polyvinyl alcohol
sponge (PVA sponge). Fig. 3a demonstrates the hydrophilicity of PVA
sponge. On contact with water, the dry PVA sponge of thickness 3 cm
rapidly absorbs water, expands in size, and is completely wetted in less
than 10 s. It should be noted that a PVA sponge of 1 cm � 1 cm X 1 cm,
on contact with water increased to dimensions of 1.2 cm � 1.2 cm X1.2
cm after complete water absorption (Fig. 3b). This shows that PVA has a
high water retention capacity. The compressibility of the PVA sponge
was also tested as shown in Fig. 3c. A completely dry PVA sponge is hard
and inelastic. No difference in thickness was visualized due to the weight
of metal block. When wetted, the sponge loses its hardness and dem­
onstrates elasticity. The thickness reduces drastically with a strain of
H.M. Wilson et al. Solar Energy Materials and Solar Cells 210 (2020) 110489

Fig. 2. a) SEM images, b) TEM image Inset SAED Pattern, c) X-ray diffraction (XRD) pattern, d) Raman spectra, e) survey scan and f) C1s spectra of spherical carbon
nanoparticles (CS).

0.47. Moreover, the durability of the sponge is high, with no visible essential for high performance solar steam generation (Fig. S5).
damage or decrease in water absorption after repeated testing. This is
beneficial in long term application of PVA sponge in solar steam gen­
3.2. Water evaporation performance evaluation
eration applications.
The last step is the attachment of CS on PVA sponge. For this purpose,
The water evaporation performance of different evaporation devices
a simple brush coating method was used. CS was first dispersed in
was evaluated using a solar simulator (Fig. 4a). The evaporation devices
ethanol to form an ethanol-CS ink. The ink was then brush coated on the
were kept under similar test conditions throughout the experimentation
top surface of the PVA sponge and dried at room temperature. The
for accurate comparison.
surface was coated till PVA sponge was dark black in color (Fig. S4). The
Fig. 4b and c shows the evaporation rates of coated PVA sponges and
attachment of CS on to PVA sponge was verified using SEM, as shown in
bare water system under 1 sun illumination. The evaporation rate of
Fig. 3(d&e). The SEM images display a uniform coating of carbon par­
bare water system was estimated to be 0.47 kg m 2 h 1 with the dark
ticles in the sponge layers. Moreover, the coating of CS on sponge has not
evaporation rate to be 0.09 kg m 2 h 1. As mentioned above, the PVA
affected the porosity of the PVA sponge which is vital for capillary action
sponges were coated only on the top surface with CS, while the other
of water. The strength of attachment of CS to the surface of the PVA was
parts of the sponge remained uncoated. In previous reports, the down­
also tested in water for stability evaluation. After repeated washing with
ward conduction losses of heat generated at the top heat zone to the
water, the CS remained attached to the surface, which can largely be
underlying bulk water have been highlighted as a primary reason for the
attributed to van der Waal’s attraction [33]. Finally, the attachment of
inferior performance of solar steam generation devices [43,44].To test
black CS on the PVA sponge also increased the solar absorption, which is
this notion, the coated PVA sponges (CPVA) were prepared and tested

4
H.M. Wilson et al. Solar Energy Materials and Solar Cells 210 (2020) 110489

Fig. 3. Digital photographs demonstrating a) the wetting of PVA sponge on contact with water. b) the increase in size of the sponge due to the excellent water
retention capacity of PVA sponge and the difference in hardness of dry PVA sponge (left) and wet PVA sponge (right). SEM images of c) Digital photographs
demonstrating the compressibility of PVA sponge when dry (left) and wet (right) respectively. d) uncoated and e) coated PVA sponges at different magnifications.

with different thicknesses (1 cm and 3 cm). It should be noted that the
coated top layer is thin with the thickness only affecting the uncoated
surface. As seen in Fig. 4c, the thickness of the PVA sponge played a vital
role in the water evaporation rate of CPVA systems. The water evapo­
ration rate increased to 1.16 kg m 2 h 1 (3 cm thickness CPVA) from
1.02 kg m 2 h 1 (1 cm thickness CPVA). The evaporation rate increases
noticeably when the thickness of the PVA sponges were varied with
higher evaporation rate with increasing thickness. This was also noticed
in the dark evaporation rates of the systems with 0.19 kg m 2 h 1 and
0.10 kg m 2 h 1 for 1 cm CPVA and 3 cm CPVA respectively. This could
be due to the additional layer of heat insulating PVA sponge in 3 cm
CPVA preventing interaction of interfacial hot spot with the underlying
bulk water and thus preventing conduction loss of heat. Meanwhile, the
evaporation rate of PVA sponge was only 0.87 kg m 2 h 1. Hence, with
the change in configuration from bare water system to substrate evap­
oration system, the evaporation rate increased by 1.85 times (PVA
sponge), 2.17 times (CPVA - 1 cm) and 2.46 times (CPVA - 3 cm) under 1
sun illumination. Since all the other parameters were constant, we can
infer that the conduction losses of heat towards underlying bulk water
affect the overall performance of the evaporation devices.
In our next test, we designed an evaporation system with cotton cloth
and polystyrene foam (C@PVA, C@CPVA) to facilitate indirect water
transport rather than encouraging direct water absorption by the
evaporation device (Fig. S6). The former method eliminates direct
contact of the evaporation device with water and also provides heat
insulation at the surface heat zone by thermally insulating polystyrene
foam. The polystyrene foam is also light-weight and hard which acts a
sturdy support to the evaporation systems. The major difference in the
C@CPVA and CPVA systems is the water path. In CPVA, the water is
absorbed by the PVA sponge directly from bulk water and transported to
the top-coated surface, where the water evaporates due to the hot zone
created by CS. In C@CPVA, the water is brought in from the two sides by
cotton cloth falling freely into the bulk water reservoir, to the heat zone
with no direct bulk fluid absorption by the PVA sponge and therefore

5
H.M. Wilson et al.
Fig. 4. a) Digital images of solar simulator and different solar evaporation systems. The water evaporation performance of b) uncoated evaporation systems and c)
camphor soot coated evaporation systems under 1 sun.
eliminating direct contact of localized hot zone with the underlying bulk
water. In experimentation, the modified capillary system showed
excellent water evaporation performance under 1 sun illumination. The
evaporation rates increased to 1.35 kg m 2 h 1 and 1.53 kg m 2 h 1 for
C@PVA and C@CPVA, respectively. These rates are 2.87 times
(C@PVA) and 3.25 times (C@CPVA) the bare water system. It is inter­
esting that even uncoated evaporation system (C@PVA) has better
evaporation rate than coated PVA systems which advocates excellent
heat localization in C@PVA and C@CPVA systems. The water vapor
temperatures were also measured during the experimentation and
C@CPVA reached a steady vapor temperature of 43 � C compared to 34
�
C of bare water system.
The performance of an evaporation system can be quantified with its
photo thermal efficiency. The photothermal efficiency can be defined as
m*ht
η¼ ; capillary water path prevents the downward conduction loss of heat to
I
where m is the effective water evaporation rate, ht is the total heat
enthalpy, and I is the intensity of solar illumination. ht is defined as ht ¼
(hvap þ 4.2 (t1 - t2); where hvap is the latent heat of vaporization with t1 -
t2 being the difference in temperature [44]. The dark evaporation rates
were subtracted from the value thus obtained, and the final effective
evaporation rates were applied as described in supporting information.
(S7-8) In 1 sun illumination, C@CPVA had the highest photothermal
efficiency of 92.38%. (Fig. 5a) The performance trend in photothermal
efficiencies were similar to their evaporation rates such as C@CPVA
(92.38%), C@PVA (80.63%), CPVA-3cm (72.1%), CPVA-1cm (56.25%),
PVA (47.77%) and bare water system (25.8%). The photothermal
6
Solar Energy Materials and Solar Cells 210 (2020) 110489
efficiency of C@CPVA is among the highest reported in literature.
(Fig. 5b) Since the solar intensities of natural sunlight vary prominently
in 0.8–1.2 suns during the day, the performance of C@CPVA was also
tested in different low solar intensities. (Fig. 5c) The C@CPVA had high
evaporation rates even at low solar intensities making C@CPVA a
promising candidate for low light passive solar applications. Further­
more, the performance of C@CPVA was tested for long term applica­
tions. As shown in Fig. 5d, C@CPVA had excellent solar evaporation
performance in repeated cycles with very little variation. This affirms
C@CPVA as an excellent solar-driven evaporation device for long-term
applications. The excellent performance of C@CPVA can be attributed
to three factors: 1) CS coated at the top layer absorbs almost all of the
incoming solar illumination due to its broadband solar absorbance. The
absorbed light is then converted to heat due to non-radiative transitions.
2) The generated heat creates a localized heat zone at the surface. 3) The
the bulk fluid preventing conduction loss of heat from heat zone to
underlying bulk fluid.
3.3. Heat localization mechanisms of different evaporation devices
The high performances of C@CPVA and C@PVA suggest that an in­
direct pathway of water to the surface heat zone is essential for highly
efficient solar-driven water evaporation. This concept was further
evaluated in detail by measuring the temperature profile of the evapo­
ration devices. For this, a thermal camera was used to record the surface
temperatures of the evaporation devices when kept under a solar
simulator for one sun illumination. The bulk water and vapor
H.M. Wilson et al.
Fig. 5. a) Comparison graph of water evaporation performance of different systems under 1 sun illumination. b) Comparison graph of photothermal efficiencies of
evaporation systems from literature with present work under 1 sun. c) Comparison graph of evaporation rates of C@CPVA system under 0.8–1.2 sun solar illu­
mination. d) The cyclic stability of C@CPVA.
temperatures were recorded simultaneously using a digital
thermometer.
Fig. 6a represents the surface temperature of different evaporation
systems. In bare water system, the surface temperature increased line­
arly from 26.4 � C to 32.3 � C in 30 min of 1 sun illumination. The tem­
perature profile is uniform from the top to the bottom of the vessel, as
seen in the thermal images (Fig. 6c). This suggests that heat was
dispersed all throughout the system. The bulk water temperature
recorded separately with digital thermometer confirmed the uniformity
in temperature from the top to the bottom of the system, as shown in
Fig. 6b. This system therefore has a dominant bulk water evaporation,
compared to surface water evaporation. This is expected, as water is a
poor absorber of solar radiation and most of the incoming light is scat­
tered in the bulk water solution.
In PVA evaporation system, the surface temperature increases non-
linearly with a surface temperature of 39 � C in 30 min (Fig. 6d). The
surface temperature increased rapidly to 32.3 � C in 2 min of solar illu­
mination. However, the temperature profiles of the evaporation system
were not linear from the top to the bottom of the system, as noted in bare
water system. In this system, the bulk water temperature showed an
increase of 6 � C in 30 min, with the temperature decreasing as we go
towards the bottom of the bulk water. Hence, we can conclude that the
bulk heating of water reduced due to the presence of PVA, while pro­
moting the surface heating of water. This explains the higher photo­
thermal efficiency of the system. Fig. 6 e &f demonstrate the surface
heating of CPVA systems. The surface temperatures of both systems viz a
viz CPVA-1cm and CPVA-3cm increase rapidly, analogous to the PVA
system, and stabilize at 40.6 � C and 39.6 � C, respectively. The overall
7
Solar Energy Materials and Solar Cells 210 (2020) 110489
temperature profiles of the evaporation systems were also non-uniform
which suggest dominant interfacial heating of water and heat localiza­
tion at the air-water interface aided by the low thermal conductivity of
CPVA (0.3 W m 1K 1). The bulk water temperatures, however, were
slightly different for both the CPVA systems. In the CPVA-1cm system,
the bulk water temperature at the top showed an increase of ~1.5 � C in
30 min. This was higher compared to the CPVA-3cm system where the
rise in bulk temperature was only ~1 � C. The increase in bulk temper­
ature suggested that localized heat at the surface was transferred to bulk
water easily once the thickness of PVA sponge increased. Thus, PVA,
being a heat insulator, decreased the downward heat conduction to bulk
water, which explains the higher photothermal efficiency of the CPVA –
3 cm system as compared to the CPVA – 1 cm system.
Fig. 6 g&h demonstrate the heat profile of capillary-based systems.
The surface temperature follows a non-linear trend on constant solar
illumination. In case of C@PVA, the surface temperature surges to 42.7
�
C in 30 min, which is higher than that of CPVA systems (Fig. 6g). The
surface temperature of C@CPVA increased non-linearly to 44.6 � C
(Fig. 6h). In both cases, the surface temperatures were higher than the
CPVA and bare water systems. The temperature profiles of the capillary
systems were comparable to the PVA systems except for the bulk water
temperatures. In C@CPVA and C@PVA systems, the bulk water tem­
perature showed no increase, owing to the indirect water path provided
in this system. The indirect water path consisting of thermally insulating
materials ie cotton and polystyrene foam having thermal conductivities
0.036 W m 1K 1 and 0.02 W m 1K 1 respectively aids in thermal
management of heat at the air-water interface. Thus, in these systems,
the bulk heating of water was nonexistent, with only the occurrence of
H.M. Wilson et al. Solar Energy Materials and Solar Cells 210 (2020) 110489

Fig. 6. a) Surface temperature variation with time for different evaporation systems. b) Variation of bulk water temperature for different evaporation systems. c, d,
e, f, g, & h) Thermal images of bare water system, PVA, C@PVA, CPVA (1 cm), CPVA (3 cm) and C@CPVA systems under 1 sun illumination in 0 min, 0.5 min, 2 min
and 30 min respectively.

Fig. 7. Schematic representation of heat loss mechanisms in various water path designs.

8
H.M. Wilson et al.
interfacial heating of water.
The thermal imaging and heat profile studies of different evaporation
systems confirm that minimizing conduction loss in a system increases
its overall photothermal performance (Fig. 7). This was quantified
mathematically with the following equation:
Q ¼ CmΔT;
where Q, C, m and ΔT represent the heat generated, specific heat ca­
pacity of water, mass of water, and rise in water temperature, respec­
tively [43]. The conduction loss for C@PVA and C@CPVA are negligible
as there is no rise in bulk water temperature. In bare water system, the
conduction loss was as high as 49.52% during experimentation. The
negligible conduction loss suggests that the capillary-based systems
have excellent heat localization at the surface. Apart from conduction
losses, radiation and convection losses are also prevalent in solar
evaporation systems. The radiation loss can be estimated using the
equation:
Q ¼ 2 σðT14 T24 Þ;
where Q, 2, σ, T1 and T2 are heat flux, emissivity, Stefan Boltzmann
constant, surface temperature, and room temperature, respectively. The
radiation loss of C@CPVA was calculated to be a meagre 1.69% [45].
Meanwhile, the convection loss of an evaporation device was calculated
using the equation:
Q ¼ hΔT
Where Q, h ¼ 10 W/m2K, ΔT where Q ¼ heat, h ¼ heat transfer coef­
ficient and ΔT ¼ tsurface - tvapor [45].
The convection loss of C@CVPA was determined to be 2.13%. The
low values of the various losses in C@CPVA confirms the excellent heat
localization of the evaporation device. The authors believe that the
performance can be further improved in a significantly optimized sys­
tem with insulation.
3.4. Application of C@CPVA in seawater desalination
Highly efficient evaporation of water is extremely valuable in solar-
driven water desalination. Here, rapid evaporation of water can be
utilized in evaporating sea-water in a solar still. Furthermore, the
generated water vapors are condensed inside the solar still to obtain
clean desalinated water. This distillation of sea-water to obtain clean
water utilizing photothermal membrane based solar-driven desalination
have been reported with extraordinary salt removal efficiencies [1,15,
29]. However, the translation of a highly efficient photothermal mem­
brane inside a working solar still for water desalination is intricate.
Several factors need to be considered while designing a solar still using
photothermal membranes. Among these factors, the arrangement of
photothermal membrane/s as a collective evaporation system is signif­
icant. The translation of an evaporation system made for solar evapo­
ration performance evaluation albeit its high efficiency-to a working
solar still is complex. This is due to the intricacy of different evaporation
systems, which achieve extremely high water evaporation rates during
solar simulator-based testing but are unrealistic in large-scale solar stills.
Moreover, the design of solar stills is imperative for the proper
condensation of the evaporated water. Hence, solar stills modified with
highly efficient evaporation systems should replicate their performance
and have the ability to be scaled quickly to large scale systems with
proper condensation of water. Fig. 8 & Fig. S9 display the authors efforts
to design such a device. As seen in the figures, an array of C@CPVA
systems was utilized in this system. For a quantitative assessment of the
solar still performance, an array of six C@CPVA systems, each having an
area of 4 cm2, was inserted into the seawater reservoir section of the
solar still. In C@CPVA water evaporation testing, the high efficiency of
water evaporation was largely due to the indirect capillary water path
9
Solar Energy Materials and Solar Cells 210 (2020) 110489
Fig. 8. Schematic representation of C@CPVA array based solar driven desali­
nation setup.
provided to the system with no contact of hot zone with the bulk water.
Similarly, in our solar still, every C@CPVA system was designed such
that it had its own indirect pathway with the sea water reservoir under
them. The seawater reservoir level was also kept low, with the only
possible contact of the evaporation systems being the cotton-based in­
direct pathway provided. Moreover, the entire reservoir area was
covered with polystyrene foam to avoid any direct bulk heating of water.
With all the above precautions, it can be assumed that the bulk heating
of water in the solar still should be minimum, with dominant interfacial
heating of seawater through C@CPVA array.
For accurate solar evaporation performance, the C@CPVA solar still
was first tested under a solar simulator. The modified solar still was kept
under different solar intensities which mimic natural direct solar in­
tensities during the day. The testing was performed for 2 h for each
intensity and the condensed water was collected and measured. The
testing was first done in identical conditions without the C@CPVA array,
which was kept as a control for comparative evaluation. Fig. 9a depicts
the comparative performance of C@CPVA solar still with bare solar still
under the incident solar intensities ranging from 0.5 sun–1 sun. In case
of the control bare solar still, no condensed water was obtained in the
collection area at 1 sun illumination. This was the case with lesser
incident solar intensities as well. The presence of minimal vapor
condensation at the top glass window suggests that the water evapora­
tion in this solar still is low (Fig. S10). This outcome is analogous to the
bare water evaporation system tested under solar simulated illumination
where the evaporation rate was subpar compared to other evaporation
systems. Meanwhile, the addition of C@CPVA array showed contrasting
results. In 1 sun illumination, the glass window was foggy within 15 min
and condensed water vapors were obtained in the collection area
(Figs. S11–12). The conditions for both bare and C@CPVA solar still
were identical and the latter produced about 3 g of water in 2 h,
compared to no water collection in the former at constant 1 sun illu­
mination. This suggests that C@CPVA replicates its high evaporation
performance when applied inside the solar still. For further evaluation of
the differences between the C@CPVA solar still and the bare solar still,
the bulk water temperatures were measured. The bulk water tempera­
ture of bare solar still increased by 3 � C in 2 h, whereas the C@CPVA
solar still had no increase in bulk water temperature. We can infer that in
bare solar still, bulk evaporation of water is dominant compared to
interfacial evaporation in C@CPVA solar still, which is assisted by in­
direct capillary water paths.
A major issue in solar stills that hinders its application for practical
purposes is its performance throughout the day. Solar stills performing
under high solar intensities require solar concentrators to maintain the
high intensities for continuous water evaporation. In photothermal-
H.M. Wilson et al.
Fig. 9. a) Sea water evaporation and condensed water collected per unit area with solar still under different solar intensities. b) Variation in amount of collected
water with change in distance of evaporation system from top glass. c) Sea water evaporation performance and condensed water collected per unit area with a solar
still under real sun. d) Thermal image of solar still at stabilized temperature condition under 1 sun illumination. (Inset) Digital photograph of the interior of the
solar still.
assisted solar stills, the systems should be able to sustain their perfor­
mance under low solar intensities. This notion was tested in C@CPVA
solar stills as illustrated in Fig. 9a. The C@CPVA solar still produced
condensed water vapors even at intensities as low as 0.5 sun illumina­
tion. The condensation of vapors at low intensities advocates the
application of C@CPVA solar stills in daylong water desalination.
The condensation of vapors into the collection area is a concern in
passive solar stills. As there is no assist by active parts, such as fans, for
the cooling of water vapors, the condensation of water is delayed. In
photothermal-based solar stills, such as C@CPVA, the C@CPVA array
floats above the water under the glass window. The generated vapors
rise up and encounter with the glass window, where they either
condense or accumulate inside the solar still until they condense to form
water droplets at the surface of the inclined glass window. The incli­
nation aids in the rolling down of the condensed vapors to the collection
area. However, this process of condensation of water vapors can be
accelerated if the distance between the glass window and C@CPVA
array is decreased. Generated water vapors immediately collide with the
glass window, restricting their movement and enhancing condensation.
This was tested in C@CPVA solar stills setup as depicted in Fig. 9b. For
these tests, the glass window and array were kept at varying distances
from each other. In 0.5 sun at a distance of 2.6 cm, about 0.12 g of water
was obtained after 2 h of constant illumination with a progressive in­
crease in collected water with increasing solar intensities. However,
when the distance was decreased to 0.6 cm, the quantity of collected
water increased greatly in all solar intensities. Even at the lowest solar
intensity of 0.5 sun, there was a 44% increase in the obtained condensed
water in comparison to that obtained at 2.6 cm. The findings reiterate
the importance of solar still design for efficient water purification
10
Solar Energy Materials and Solar Cells 210 (2020) 110489
applications.
Thus, we confirmed that the performance of C@CPVA solar stills is
superior even at low solar intensities. However, since the performance
evaluations were done under constant illumination and laboratory test
conditions, the C@CPVA solar still was further tested under natural
sunlight for evaluating potential practical applications (Fig. S10). In this
experimentation, the solar still was kept in natural sunlight from 10 a.m.
to 4 p.m. For variability in test conditions, the testing was conducted in a
sunny day and a cloudy day (Fig. 9c and d). In both days, the solar still
successfully evaporated sea water and generated condensed water. We
would like to reiterate that no solar concentrators were utilized during
experimentation and the solar still was kept untouched throughout the
experimentation period. The obtained condensed water was therefore a
product of natural solar intensities incident on the still during the test
period. This confirms the practical applicability of C@CPVA solar stills
under natural sunlight with unfocussed solar intensities. The efficacious
distillation of seawater with the solar still has been confirmed under
natural sunlight. Yet, for water desalination application, the condensed
water sample should have low salinity. The salinity levels of seawater
and obtained condensed water samples were tested in each experi­
mentation. The salinity levels of seawater decreased by 99.9% to less
than 200 ppm in condensed water sample. Hence, from the above re­
sults, it is confirmed that C@CPVA solar still is an excellent device for
solar-driven desalination. The performance of the solar still under nat­
ural, non-concentrated solar intensities advocates their potential use in
practical, real life applications. Moreover, the facile design of the solar
still and the C@CPVA systems aids in the rapid scaling of the system for
large-scale applications.
H.M. Wilson et al.
4. Conclusion
In summary, we have fabricated a novel, facile, and low cost device
using plant-derived carbon nanoparticles to produce excellent solar-
driven steam generation and low intensity solar desalination. The
design of the evaporation system primarily involved commonly avail­
able and abundant materials, endorsing ease in scalability for large-scale
systems. The novel C@CPVA evaporation system produced steam at a
rate of 1.53 kg m 2 h 1 under 1 sun illumination with an outstanding
photothermal efficiency of 92.38% due to its indirect capillary pathway
design. The C@CPVA evaporation system was further applied as an
array for solar-driven water desalination application. A simple C@CPVA
solar still condensed seawater to generate clean water at substantially
low solar intensities with high salt removal efficiency. The excellent
performance of our solar still setup provides up opportunities for further
research on facile, scalable passive solar stills for long term utilization
under non-concentrated natural sunlight utilization.
Author contribution
Higgins M. Wilson- Conceptualization, Methodology, Data curation,
Investigation, Visualization, Writing- Original Draft preparation.
Tushar- Methodology, Data curation, Visualization, Investigation,
Editing.
Shakeelur Raheman AR- Investigation, Reviewing.
Neetu Jha- Reviewing, Supervision.
Acknowledgement
The authors acknowledge the financial support by University grants
commission of India (UGC-MANF) and Science and Engineering
Research Board (SR/FTP/PS-045/2012).
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.solmat.2020.110489.
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