Article

Storage and Recycling of Interfacial Solar

Steam Enthalpy
Xiuqiang Li, Xinzhe Min, Jinlei
Li, ..., Bin Zhu, Shining Zhu, Jia
Zhu
jiazhu@nju.edu.cn

HIGHLIGHTS
Steam enthalpy is stored and
recycled from interfacial solar
steam process

This solar device can produce

water and electricity
simultaneously

The integrated thermal storage

enables power generation after
sunset

This integrated system combines

solar energy conversion, storage,
and utilization

By using solar energy and sea (or contaminated) water, abundant resources on
Earth, this solar device can generate clean water and electricity simultaneously,
through storing and recycling the steam enthalpy derived from the interfacial solar
steam-generation process. In addition, the integrated capability of thermal
storage can enable electricity generation over an extended period after sunset.
Combining conversion, storage, and utilization, this integrated solar energy
device can provide the basic needs in various off-grid and/or resource-constrained
areas.

Li et al., Joule 2, 2477–2484

November 21, 2018 ª 2018 Elsevier Inc.
https://doi.org/10.1016/j.joule.2018.08.008
Article
Storage and Recycling of Interfacial
Solar Steam Enthalpy
Xiuqiang Li,1,2 Xinzhe Min,1,2 Jinlei Li,1 Ning Xu,1 Pengchen Zhu,1 Bin Zhu,1 Shining Zhu,1
and Jia Zhu1,3,*

SUMMARY Context & Scale

In this work, it is shown that by storing and recycling steam enthalpy derived Interfacial solar steam generation
from the solar steam process, we can enable simultaneous generation of clean has recently demonstrated great
water and electricity. Energy-transfer efficiency of solar to steam can reach potential in various applications,
72.2% with extra electricity power (with 1.23% efficiency) generated simulta- from desalination and distillation
neously. With advanced thermal management to further elevate the working to catalysis. However, in most
temperature and exciting progress in the fields of thermoelectrics and desalina- previous studies the steam
tion, it is expected that the performance of this system can be further improved. enthalpy was typically lost to the
This approach with scalable materials and processes, high energy-transfer effi- environment during condensation
ciency, and integrated storage capability will provide an attractive avenue to without any utilization. In this
produce electricity and clean water in an individualized manner, particularly work, we demonstrate that
desirable in various off-grid areas. through designs and integrations
of materials and systems, steam
INTRODUCTION enthalpy can be stored and
recycled for power generation (at
Clean water and electricity, essential to the daily life of humans, are unfortunately
efficiency of 1.23%), in addition to
scarce resources in various parts of the world, especially in developing countries
72.2% solar-to-vapor efficiency. In
and remote areas.1–3 Interfacial solar steam generation4–34 has demonstrated great
addition, the integrated capability
potential in various fields such as desalination,4–7 waste-water treatment,8,9 and
of thermal storage can enable
electricity generation.10 In previous studies, high energy-transfer efficiency from so-
electricity generation over an
lar to steam has been demonstrated through rational designs of material struc-
extended period after the light
tures,8,11 photon management,5,12 heat localization,13 and water supply.4,9 In
source is turned off. Combining
most if not all of the previous studies of interfacial solar steam generation, the inter-
solar energy conversion, storage,
nal enthalpy of steam is usually lost to the environment as steam condenses to form
and utilization, this method based
water (Figure 1A). Recently, Zhou’s group demonstrated the concept of simulta-
on low cost and scalable graphite/
neous generations of steam and electricity (1 W/m2 under one-sun illumination,
nonwoven films provides a
0.1% efficiency) by taking advantage of the evaporation-induced salinity
complementary system to
gradient.10 A significant increase in power generation is expected to open up
produce clean water and
tremendous opportunities. In this work, by storing and recycling the internal
electricity, the basic needs in
enthalpy of steam during steam condensation, we demonstrate simultaneous gen-
various resource-constrained
eration of clean water (72.2% efficiency) and electricity (1.23% efficiency) with solar
areas.
energy as the only energy input (Figure 1B). In addition, the integrated capability of
thermal storage enables the generation of electricity over an extended period after
the light is extinguished, as illustrated in more detail below.

RESULTS AND DISCUSSION

The storage and recycling of interfacial solar steam enthalpy for simultaneous gen-
eration of clean water and electricity is shown in Figure 1B (the real setup is shown in
Figure S1). This high-temperature steam generated by an interfacial solar steam
generator (as shown in Figure S1A) flows into the area of thermal storage and water
generation, with an aluminum chamber wrapped by a polyurethane foam (as shown

Joule 2, 2477–2484, November 21, 2018 ª 2018 Elsevier Inc. 2477

Figure 1. Schematic of the Condensation Processes of Interfacial Solar Steam Generation
(A) Traditionally, steam condenses to form water with enthalpy lost to the environment.
(B) Storage and recycling of interfacial solar steam enthalpy for simultaneous generation of clean
water and electricity.

in Figure S1B) for thermal insulation. Because of the heat exchange between high-
temperature steam and the chamber, steam will be condensed to produce clean
water at the outlet of the chamber, while the energy in the steam is reserved in
the chamber to maintain it at a high temperature. The temperature gradient formed
between this chamber and the room-temperature environment can then be used
for electricity generation by using the thermoelectric modules (based on Bi2Te3
materials; for more details see Experimental Procedures).

The device performance depends on the properties of the solar absorber.

Currently there are mainly two categories of nanomaterials for solar steam gener-
ation, namely carbon-based and plasmonic-based absorbers. Here, graphite/
nonwoven film is selected as a solar absorber of interfacial solar steam generation
mainly because it has efficient absorption, excellent stability and foldability, and
can be fabricated through a scalable and cost-effective process. All of these fea-
tures are detailed below. The graphite/nonwoven absorber can be conveniently
fabricated by spraying the ethanol solution of graphite toward a piece of pre-
heated nonwoven material (for more details see Experimental Procedures); corre-
sponding optical images of nonwoven fabric (10 cm 3 5 cm) before and after
spray-coating are shown in Figures 2A and 2C. The corresponding scanning elec-
tron microscopy (SEM) images are shown in Figures 2B and 2D, which demonstrate
clearly the graphite particles (size about a few hundred nanometers) on nonwoven
fibers. This graphite/nonwoven film has efficient and broadband absorption, with
about 98% weighted absorption (by standard AM 1.5G solar spectrum) from
250 nm to 2,500 nm (Figure 2E). Another unique property of this graphite/
nonwoven film is that it can maintain its integrity when immersed in water and
1National Laboratory of Solid State
even after shaking for a long time (Figures 2F and 2G), which is beneficial for
Microstructures, College of Engineering and
practical applications. Moreover, the absorber can be easily folded because of Applied Sciences, School of Physics, Key
the flexible nonwoven substrates (as shown in Figure S2), advantageous for Laboratory of Intelligent Optical Sensing and
Integration, and Collaborative Innovation Center
large-scale carriage and deployment. of Advanced Microstructures, Nanjing University,
Nanjing 210093, P.R. China
2These
The mass change over time under different solar concentrations is shown in Fig- authors contributed equally
3Lead
ure 3A. In the beginning, the mass change is not obvious within first few minutes Contact
(for example, 2 min under illumination of 30 kW/m2) because of the initial inner *Correspondence: jiazhu@nju.edu.cn
condensation of steam in the solar steam-generation device. Thereafter it starts to https://doi.org/10.1016/j.joule.2018.08.008

2478 Joule 2, 2477–2484, November 21, 2018

Figure 2. Solar Absorbers Based on Graphite/Nonwoven
(A and B) Optical image (A) and SEM image (B) of nonwoven material.
(C and D) Optical image (C) and SEM image (D) of graphite/nonwoven.
(E) Absorption spectrum of graphite/nonwoven from 250 to 2,500 nm.
(F) Optical image of graphite/nonwoven in water.
(G) Optical image of graphite/nonwoven in water after shaking 50 times.

show the nearly linear mass change over time under 30 kW/m2, which is orders of
magnitude shorter than that of the traditional bulk water heating (around 20 min,
see Figure S3). That is a direct indication of much reduced heat loss for interfacial
heating and therefore reduced time to reach a steady state. As shown in Figure 3B,
the temperature of steam can reach a steady state after 666 s, 146 s, 40 s, and 32 s
under 8, 17, 22, and 30 kW/m2, respectively, which is also an indication of reduced
time response of interfacial heating. The formula h = mhLV/Pin is used for calculating
the solar-to-steam efficiency (h), where m is the mass flux, hLV is total liquid-vapor
phase-change enthalpy (phase-change enthalpy + sensible heat), and Pin is the
received power density of the solar irradiation on the absorber surface.13 As shown
in Figure 3C, the evaporation rates (obtained from the slope of the mass change
curves at steady state) are 4.2, 15.5, 24.3, and 34.8 kg/m2 h under 8, 17, 22, and
30 kW/m2, respectively, and corresponding efficiencies are 36.4%, 64.7%, 73.3%,
and 81.7%, respectively. It should be noted that this efficiency is achieved in a
semi-closed system that is different from earlier reported efficiency in an open sys-
tem (for more details see Supplemental Note 1). This increased trend of efficiency

Joule 2, 2477–2484, November 21, 2018 2479

Figure 3. Interfacial Solar Steam Generation
(A) Mass change over time of interfacial solar steam generator under different solar irradiations.
(B) Temperature of output steam over time under different solar irradiations.
(C) Dependence of evaporation rate and corresponding efficiency on optical concentrations. Error
bars indicate the SD of the measurements.
(D) Concentrations of various metal ions before and after treatment (the blue line refers to the WHO
standards for drinking water).

with increased power input is consistent with previous studies,5,13 and can be
ascribed to the decreasing ratio of heat loss under higher illumination (for more de-
tails about thermal analysis see Supplemental Note 2). As shown in Figure S4, the
evaporation rates with integrated thermal storage are 3.0, 14.5, 21.7, and
31.6 kg/m2 h under 8, 17, 22, and 30 kW/m2, respectively, with corresponding effi-
ciencies of 26.5%, 60.5%, 70.0%, and 74.7%, respectively. The clean water can be
collected once the steam is condensed, even directly from contaminated water sour-
ces. As an example of demonstration, water contaminated with rich Pb2+, Cu2+, and
Cr3+ ions, common heavy metal pollutants, is used. As shown in Figure 3D, the result
shows that the output water (the Pb2+, Cu2+, and Cr3+ ion concentration 0.007,
0.338, and 5 3 10 4 mg/L, respectively) can reduce the metal ion concentrations
by two orders of magnitude, and meet the World Health Organization (WHO) drink-
ing water standard (Pb2+: 0.01 mg/L; Cu2+: 2 mg/L; Cr3+: 0.05 mg/L).35

With the chamber temperature of the thermal storage area maintained at 100 C and
room temperature (25 C), the thermoelectric module can be used for electricity
generation. The output of the thermoelectric module is highly dependent on the
temperature difference on its two sides. Once the light source is turned on, both
the open-circuit voltage and short-circuit current will first increase as the chamber
temperature increases until reaching the steady state at around 100 C, as shown
in Figures 4A and 4B (corresponding temperatures of hot side and cool side are
shown in Figure S5). With the increased solar power illumination, a larger amount
of steam will be generated to transfer more condensation latent heat to the
thermoelectric module, therefore further enhancing the open-circuit voltage and
short-circuit current, up to 3.87 V and 0.55 A under 30 kW/m2.

2480 Joule 2, 2477–2484, November 21, 2018

Figure 4. Performance of Electricity Generation
(A) Open-circuit voltage over time under different solar irradiations.
(B) Short-circuit current over time under different solar irradiations.
(C) Maximum output power of the thermoelectric device under different solar irradiations.
(D) Optical image of an operating electric fan and an illuminating light-emitting diode powered by
interfacial solar steam generation. A movie showing simultaneous generations of electricity and
clean water is provided in Video S1.

Figure 4C shows the output power of the thermoelectric device under different solar
irradiations. We found that the maximum output power was achieved when external
resistance is about 6 U and output power is 1.7, 135.7, 363.0, and 574 mW under 8,
17, 22, and 30 kW/m2, respectively, with corresponding output power density of 0.9,
69.2, 185.2, and 292.9 W/m2, respectively. The formula h = Pe/Pin is used for calcu-
lating the power generation efficiency (h), where Pe and Pin are the output energy of
power generation and input energy of solar. It can be seen that the maximum effi-
ciency can reach 0.98% under 30 kW/m2 (energy analysis is detailed in Supplemental
Note 2). The efficiency can be further enhanced by increasing the steam temperature
using techniques such as superheated steam (for more details see Supplemental
Note 3). It can be seen that the open-circuit voltage and short-circuit current can
reach to 4.15 V and 0.61 A, while the maximum efficiency can reach 1.23% under
30 kW/m2 (comparison with solar cell-based technology is detailed in Supplemental
Note 4). Therefore various applications can be supported, such as continuous oper-
ation of an electric fan (1 W) and 28 light-emitting diodes (total power 1.5 W), as
shown in Figure 4D. Given advanced thermal management to further increase the
steam temperature and exciting progress in the field of thermoelectrics and solar
desalination, it is expected that the performance of this system can be further
improved (more analysis is provided in Supplemental Note 5).

In addition to simultaneous generation of purified water and electricity, another

unique feature of this device is that it has integrated thermal storage, which can
enable power generation over an extended period without sunlight. After the light
source is turned off, the polyurethane foam-wrapped aluminum chamber with ther-
mal capacity will release sensible heat to maintain electricity generation, as shown in
Figures 4A and 4B (for a movie of continuous generation of electricity without

Joule 2, 2477–2484, November 21, 2018 2481

sunlight, see Video S2). The duration of the extended period can be tuned by
thermal capacity or mass of chapter materials (for more analysis see Supplemental
Note 6), which can be used to reduce the influence of intermittent illumination
such as rolling cloud cover (for more details see Supplemental Note 7). The perfor-
mance is expected to be further promoted by employing phase-change materials
that can tune the mismatch between solar illumination and power usage.

Conclusions
This work shows that by storing and recycling steam enthalpy derived from the so-
lar steam process, we can enable simultaneous generation of clean water and elec-
tricity. The results showed that the energy-transfer efficiency of solar to steam can
reach 72.2% with extra electricity power (with 1.23% efficiency) generated simulta-
neously (a comparison with solar cell-based technology is provided in Supple-
mental Information). With advanced thermal management to further elevate the
working temperature and exciting progress in the field of thermoelectrics and solar
desalination, it is expected that the performance of this system can be further
improved (for more analysis see Supplemental Information). This approach with
scalable materials and processes, high energy-transfer efficiency, and integrated
storage capability will provide an attractive avenue through which to produce elec-
tricity and clean water in an individualized manner, particularly desirable in various
off-grid areas.

EXPERIMENTAL PROCEDURES
Fabrication of Solar Absorbers (Graphite/Nonwoven Film)
Graphite particles with diameter of about 30 nm were dispersed in ethanol solution
at the concentration of 5 mg/mL followed by 2 hr of ultrasonication. The graphite
solution was then sprayed through a commercial airbrush (nozzle diameter
0.3 mm; Ustar CD-601, Taiwan) toward the preheated nonwoven to produce
graphite/nonwoven film.

Interfacial Solar Steam-Generation Device

Hydrophilic nonwoven-wrapped polystyrene foam (about 2 cm thick, as water supply
layer and thermal insulation layer) was floated on the surface solution in a beaker with
an insulation layer. A graphite/nonwoven film was placed on the surface of
nonwoven-wrapped polystyrene foam. A transparent quartz plate covered the up-
per surface of the beaker while a thermal insulated tube was connected inside the
beaker.

Electricity Generation Setup

As shown in Figure S1, the commercial thermoelectric module (Bi2Te3, length 8 cm,
width 4 cm, height 3.4 mm, ZT about 1 at 373 K) was selected as the power gener-
ation device. The cool side was connected to a cooling fin placed in water and the
hot side was connected to a two-end open insulation chamber.

Characterizations
The morphologies and structures of the solar absorber (graphite/nonwoven) were
characterized by a scanning electron microscope ( Dual-beam FIB 235; FEI Strata).
The absorption of graphite/nonwoven was measured from 200- to 2,500-nm wave-
length using a UV-visible spectroscope (UV-3600; Shimadzu). The concentration of
heavy metal ions was characterized by ICP-OES (0.1 mg/L accuracy, PTIMA 5,300
DV; PerkinElmer Instruments).

2482 Joule 2, 2477–2484, November 21, 2018

Simultaneous Generations of Electricity and Clean Water
The device was irradiated by a xenon lamp (HSX-F300; Excelitas). The temperature
of the steam was recorded by thermocouples (placed in insulated tube, as shown in
Figure S1A, T1). The temperature of the hot side of the thermoelectric module
was recorded by thermocouples (placed in an aluminum chamber, as shown in
Figure S1B, T2 and T3). The mass change was monitored by electronic analytical
scale, recorded in real time by the computer (with RS-232 serial ports) and used to
determine the mass change of solar steam generation. The open-circuit voltage
and short-circuit current was recorded by a multimeter. The power line was obtained
by changing the external resistance.

SUPPLEMENTAL INFORMATION
Supplemental Information includes Supplemental Experimental Procedures, 11 fig-
ures, and 2 videos and can be found with this article online at https://doi.org/10.
1016/j.joule.2018.08.008.

ACKNOWLEDGMENTS
We acknowledge the micro-fabrication center of the National Laboratory of Solid
State Microstructures for technical support. This work is jointly supported by the Na-
tional Key Research and Development Program of China (no. 2017YFA0205700) and
the State Key Program for Basic Research of China (no. 2015CB659300), National
Natural Science Foundation of China (nos. 11621091, 11574143, 61735008), and
the Fundamental Research Funds for the Central Universities (nos. 021314380135,
021314380128).

AUTHOR CONTRIBUTIONS
J.Z., X.L., and X.M. designed research; X.L. and X.M. performed research; J.L., N.X.,
P.Z., and B.Z. contributed new reagents/analytical tools; X.L., X.M., S.Z., and J.Z.
analyzed data; X.L., X.M., and J.Z. wrote the paper.

DECLARATION OF INTERESTS
The authors declare no competing interests.

Received: November 22, 2017

Revised: April 17, 2018
Accepted: August 17, 2018
Published: September 7, 2018

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JOUL, Volume 2

Supplemental Information

Storage and Recycling of Interfacial

Solar Steam Enthalpy
Xiuqiang Li, Xinzhe Min, Jinlei Li, Ning Xu, Pengchen Zhu, Bin Zhu, Shining Zhu, and Jia
Zhu
 Supplemental Information

Figure S1. Photos of the real setup

Figure S1. Photos of the real setup. (A) Optical image of steam generation device. (B) Optical image of

electricity and water generations. (Inset) The optical of aluminum chamber without top plate. The

aluminum chamber (Length: 11 cm, Width: 5.5 cm, Height: 1 cm) was selected as condensed chamber.

Some yellow copper wire was filled in the inside of aluminum chamber to increase steam condensation.

T1, T2 and T3 represent the position of thermocouples.

1
Figure S2. Optical images of folded and unfolded graphite/nonwovens films

Figure S2. Optical images of folded and unfolded graphite/nonwovens film. (A) Optical image of a folded

graphite/nonwovens film. (B) Optical image of an unfolded graphite/nonwovens film after folding over

50 times.

2
Figure S3. Comparison of interfacial heating and bulk heating

Figure S3. Comparison of interfacial heating and bulk heating. (A) The mass change over time at bulk

heating and interfacial heating under 30 kW/m2. (B) Steam temperature over time at bulk heating and

interfacial heating under 30 kW/m2.

3
Figure S4. The influence of thermal storage part on performance of solar steam generation

Figure S4. Mass change over time of interfacial solar steam generator with thermal storage part under

different solar irradiations.

4
Figure S5. The temperature distribution in thermoelectric device

Figure S5. The temperature distribution in thermoelectric device. (A), (B), (C) and (D) temperature

distribution in thermoelectric device under 8, 17, 22 and 30 kW/m2 respectively. (Hot (in) represents the

temperature of hot side near steam; Hot (out) represents the temperature of hot side near water outside;

Cool represents the cool side of thermoelectric device.

5
Supplemental Note 1.Comparison of open system and semi-closed system

Interfacial solar steam was proposed and achieved high efficiency ( ~ 80%) under one sun with advanced

structure and material designs, photon and thermal management, including our group 1,2. However, this

efficiency is achieved in open system that is different from all the previous systems, which is a semi-

closed system. Here, a set of comparative tests were made to support this point. As shown in Fig. S6, the

efficiency of our solar steam generator can reach around 75% under one sun if we remove sealed cap,

but only about 18% efficiency in semi-closed system under one sun. The possible reason is that the vapor

diffusion is suppressed that resulted in the decrease of evaporation rate in semi-closed system.

Figure S6. The difference of open system and semi-closed system. (A) The schematic of open system

and semi-closed system. (B) The evaporation rate (Note: The evaporation rate represents the rate, which

subtract dark evaporation rate) of open system and semi-closed system over time under 1 kW/m2.

6
Supplemental Note 2. The analysis of energy loss

The heat loss by the solar steam generator consist of three losses: radiation, convection and conduction.

Here, the radiation loss was calculated by Stefan- Boltzmann.

Φ ＝εA σ(T14-T24) (1)

Where Φ denotes heat flux, ε is emissivty (assuming the absorber has maximum emissivity of 1), A is

surface area (about 20 cm2), σ is Stefan- Boltzmann constant, T1 is the average temperature of absorber

(The temperature of absorber are 100℃, 100℃, 100℃ and 100℃ under 8, 17, 22 and 30 kW/m2,

respectively) and T2 is an environmental temperature (~25 ℃) in the experiment. Therefore, based on

equations (1), the radiation heat losses of solar steam generator have account for 8%, 4%, 3% and 2%

under 8, 17, 22 and 30 kW/m2, respectively.

The convection loss was calculated by Newton' law of cooling.

Q= h A (T1-T2) (2)

Where Q denotes the heat, h is convection heat transfer coefficient (10 W/m2K). A is surface area (The

area of glass sealed cap is about 50 cm2) and T1 is the temperature of glass sealed cap. ( The temperature

of glass sealed cap are 98 ℃, 122 ℃, 144 ℃ and 157 ℃ under 8, 17, 22 and 30 kW/m2, respectively)

and T2 is an environmental temperature (~25 ℃) in the experiment. Therefore, based on equations (2),

the convection heat losses of solar steam generator have account for 19%, 14%, 13% and 11% under 8,

17, 22 and 30 kW/m2, respectively.

The conduction loss was calculated by Fourier's law.

Φ = -kA▽T (3)

Where Φ denotes the heat flux, k is the thermal conductivity of material (0.04 W/mK), A is the area

7
(about 20 cm2) and ▽T is temperature gradient. The temperature of absorber are 100 ℃, 100 ℃, 100 ℃

and 100 ℃ under 8, 17, 22 and 30 kW/m2 respectively, and T2 is an environmental temperature (~25 ℃)

in the experiment. The thickness of material is about 1.3 cm. Therefore, based on equations (3), the

conduction losses of solar steam generator have account for 3%, 1%, 1% and 1% under 8, 17, 22 and 30

kW/m2, respectively.

It is note that the optical losses are 10% (5% come from absorber and the other 5% come from glass

sealed cap). We noted that the heat losses and efficiency have a big discrepancy under 8 kW/m2. The

possible reason is that there are some condensed water on the glass sealed cap (as shown in Fig. S7) that

increase the optical reflection3. Obviously, the ratio of heat losses is decreasing under higher illumination

(The heat losses are 14% ,17%, 19% and 30% under 30, 22, 17 and 8 kW/m2, respectively).

Figure S7. The phenomenon of condensation on the sealed cap. (A) The phenomenon of condensation

on the sealed cap under 8 kW/m2. (B) The phenomenon of condensation on the sealed cap under 17

kW/m2.

It can be found that about 25% energy has lost in the process of solar energy to steam generation under

30 kW/m2. In other words, about 75% energy was used for power generation. Obviously, most energy as

heat loss was wasted instead of using for power generation. Here, the thermal conductivity of insulation

foam and thermoelectric materials are about 0.04 and 1.5 W/mK. The thickness of insulation foam and

8
thermoelectric materials are about 1.6 cm and 0.4 cm. The area of insulation foam and thermoelectric

materials are about 122 cm2 and 32 cm2. Based on Fourier's law, we can calculate the ratio of heat losses

through the insulation foam and thermoelectric materials are about 1.9% and 72.1%.

9
Supplemental Note 3. The superheated steam for simultaneous generations of clean water and electricity

In order to further enhance the performance of simultaneous generations of clean water and electricity,

the superheated steam method was selected to increase the steam temperature. As shown in Figure S8-

1A, a black Cu tube (diameter 5 mm), which was placed between absorber and sealed glass, was selected

as heating body to further heat the steam to achieve the superheated steam. The schematic diagram of

superheated steam generation device is showed in Figure S8-1B. The black Cu tube can reach high

temperature (>100 ℃) under illumination of the sun. Then, the black Cu tube can heat the steam to

superheated steam when the steam flow through the black Cu tube.

Figure S8-1. The schematic diagram of superheated steam generation device. (A) Optical image of

superheated steam generation device. (B) The schematic of superheated steam generation device.

The mass change over time under 30 kW/m2 is shown in Figure S8-2A. The efficiency of superheated

steam generation device is about 72.2% (obtained from the slope of the mass change curves at steady

state). More strikingly, the temperature of steam is larger than 100 ℃, and can reach 146 ℃ at steady

state under 30 kW/m2 (as shown in Figure S8-2B). It can be seen that the open-circuit voltage and short-

circuit current can reach to 4.15 V and 0.61 A, and the maximum efficiency can reach 1.23% under 30

kW/m2 (as shown in Figure S8-2C and D). In the future, it is expected that advanced thermal control and

10
management can be used to further increase the steam temperature, and therefore to further improve the

power generation performance.

Figure S8-2. The performance of superheated steam generation device. (A) Mass change over time of

superheated steam generation device under illumination of 30 kW/m2. (B) Temperature of output steam

over time under illumination of 30 kW/m2. (C) Voltage and current over time under illumination of 30

kW/m2. (D) Output power over resistance under illumination of 30 kW/m2.

11
Supplemental Note 4. Comparison with solar cell based technology

Let’s use solar cell (20% solar to electricity efficiency) and solar desalination membrane (95% solar to

vapor efficiency). As shown in Fig. S9, for one square meter of light, the total conversion efficiency

should range from 20% (if one square meter area is covered with solar cell) to 95% (if one square meter

area is used only for solar desalination membrane). For example, if we use 0.5 sqm for solar cell and 0.5

sqm for solar desalination, the total efficiency is 57.5% (20 × 0.5 + 95 × 0.5 = 57.5%) or equivalent to

the efficiency of 10% for solar to electricity and 47.5% for solar to vapor. If we use 0.1 sqm for solar cell

and 0.9 sqm for solar desalination, the total efficiency is 87.5% (20 × 0.1 + 95 × 0.9 = 87.5%) or

equivalent to the efficiency of 2% for solar to electricity and 85.5% for solar to vapor.

Figure S9. The comparison of efficiency between solar cell + solar still and our device.

For comparison, as shown in Fig. S9, for the same one square meter of light, our device can generate

~72.2% for solar to steam and ~1.23% for solar to electricity, as the electricity is generated by recycling

the internal energy of steam from solar steam process.

With quantitative explanations above, it clear that in terms of efficiency, our device is comparable to PV

powered approach while it is still at infancy.

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Supplemental Note 5. Future improvement

The device can be further developed and optimized, with the advances in the field of solar steam

generations and thermoelectrics. For example, we are pleased to see 95% solar-to-steam conversion

efficiency was achieved through the design of hydrogels recently4, which can be used to further improve

the efficiency of our concept. Tremendous progress has also been made in the field of thermoelectrics.

The thermoelectric device efficiency can be expressed as:

T 1  ZTavg  1
 (1)
Th 1  ZT  Tc
avg
Th

Where η is thermoelectric device efficiency. A theoretical quantitative analysis reveals that with solar to

steam efficiency of 95% and ZT=2 at 400 K, we can expect ~95% solar to steam and 7.9% solar to

electricity. With solar to vapor efficiency of 95% and ZT=2.5 at 400 K, we can expect ~95% solar to

vapor and 8.9% solar to electricity, which will then be much higher compared to what you can achieve

with solar cell powered approach (as in Fig. S9).

13
Supplemental Note 6. Analysis of the integrated thermal storage

The relationship between thermal storage ability and time evolution of output is analyzed. In our

experiment system, the heat flow is assumed to travel just through thermoelectric module because the

chapter is wrapped by thermal insulation materials. Meanwhile, the conversion efficiency of

thermoelectric module is assumed to be a constant. We can obtain the following formulas:

T0 - Tt
P( t )  P0 (1)
T0  Te

P(t)  Qf (t ) (2)

Qf (t )dt  -cmdT (3)

Temperature and output power can be produced as following,

P0 t
-
(T0 Te )cm
T ( t )  Te  (T0  Te )  e (4)
P0 t
-
P( t )  P0  e (T0 Te )cm (5)

P is output power. T0 and Te are steady temperatures under irradiation and temperature of environment,

respectively. P0 is the initial output power. Qf is the heat flux through the thermoelectric module. η is the

conversion efficiency of thermoelectric module. c and m are thermal capacity and mass of chapter. In the

experiment, T0=100 ℃, Te=25 ℃, P0=0.208 W, Qf=37 W, c=0.88 J/g℃, m=75 g. Hence,

t
-
P(t )  0.209  e 130.26 (6)

The relationship between thermal storage ability and performance of output power is shown in Fig. S10.

14
Figure S10. The relationship between output power (P) and thermal storage of the chamber. (A) P/P 0

over C/C0 (where P0 represents steady output power under irradiation, and P represents output power of

1 min after tuning off the light. C0=cm, where c and m are thermal capacity and mass of chapter in this

experiment). (B) P/P0 over time at different thermal storage capabilities.

15
Supplemental Note 7. Power generation performance of device under discontinuous irradiation

The duration of the extended period can be used to reduce the influence of intermittent illumination such

as rolling cloud cover. As shown in Fig. S11A and B, discontinuous irradiation (in each cycle, the interval

is 1 min between on and off) was used to simulate changing cloud cover in real applications. It can be

seen that the device with thermal storage can continually output electricity. That speciality is determined

by thermal storage ability of chapter and can be promoted by tuning thermal capacity or mass of chapter

materials. As shown in Fig. S10A, the reduction of output power is only about 10 % decrease when the

thermal storage increase 5x.

Figure S11. Power generation performance of device under discontinuous irradiation. (A) The change of

open-circuit voltage with/without solar irradiation under 30 kW/m2. (B) The change of short-circuit

current with/without solar irradiation under 30 kW/m2.

16
References

[1] Li, X., Xu, W., Tang, M., Zhou, L., Zhu, B., Zhu, S., Zhu, J. (2016). Graphene oxide-based efficient

and scalable solar desalination under one sun with a confined 2D water path. Proc. Natl. Acad. Sci. USA

113, 13953-13958.

[2] Hu, X., Xu, W., Zhou, L., Tan, Y., Wang, Y., Zhu, S., Zhu, J. (2017). Tailoring graphene oxide-based

aerogels for efficient solar steam generation under one sun. Adv. Mat. 29, 1604031.

[3] Zhu, K., Huang, Y., Pruvost. J., Legrand. J., Pilon. L. (2017). Transmittance of transparent windows

with non-absorbing cap-shaped droplets condensed on their backside. Journal of quantitative

spectroscopy and radiative transfer 194, 98-107.

[4] Zhao, F., Zhou, X., Shi, Y., Qian, X., Alexander, M., Zhao, X., Mendez, S., Yang, R., Qu, L.,& Yu, G.

(2018). Highly efficient solar vapour generation via hierarchically nanostructured gels. Nature

nanotechnology, doi:10.1038/s41565-018-0097-z.

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