DOI: 10.1002/cssc.
201500848 Full Papers
Life Cycle Assessment of Titania Perovskite Solar Cell
Technology for Sustainable Design and Manufacturing
Jingyi Zhang,[a] Xianfeng Gao,[a] Yelin Deng,[a] Bingbing Li,[b] and Chris Yuan*[a]
Perovskite solar cells have attracted enormous attention in
recent years due to their low cost and superior technical per-
formance. However, the use of toxic metals, such as lead, in
the perovskite dye and toxic chemicals in perovskite solar cell
manufacturing causes grave concerns for its environmental
performance. To understand and facilitate the sustainable de-
velopment of perovskite solar cell technology from its design
to manufacturing, a comprehensive environmental impact as-
sessment has been conducted on titanium dioxide nanotube
based perovskite solar cells by using an attributional life cycle
assessment approach, from cradle to gate, with manufacturing
data from our laboratory-scale experiments and upstream data
Introduction
With the high demand for energy usage, perovskite sensitized
solar cells have attracted enormous attention in recent years
due to their low cost and superior technological advantages.[1]
Perovskite dye shows remarkable optical absorptions over
a broader range, which enables efficient light harvesting in
very thin films.[2] Moreover, they exhibit long charge-carrier dif-
fusion lengths (> 1 mm) relative to the absorption depth of in-
cident light (100 nm),[3] which means that almost all photoex-
cited species in perovskite are able to reach the charge-collec-
tion electrodes and results in superior performance. The theo-
retical maximum power conversion efficiency (PCE) of perov-
skite solar cells can reach 30 %.[4] In current research, two types
of perovskite solar cells have been developed by using liquid
and solid-state electrolytes with PCE values of around 7 and
20 %, respectively.[5]
Research progress has revealed that perovskite solar cells
have a promising future in replacing expensive silicon and cad-
mium–tellurium thin-film photovoltaic (PV) technologies cur-
rently commercially available.[6] With the rapid development of
[a] J. Zhang, Dr. X. Gao, Dr. Y. Deng, Dr. C. Yuan
Department of Mechanical Engineering
University of Wisconsin—Milwaukee
3200 N Cramer, Milwaukee, WI, 532211 (USA)
E-mail: cyuan@uwm.edu
[b] Dr. B. Li
Department of Manufacturing System Engineering & Management
California State University—Northridge
18111 Nordhoff Street, Northridge, CA, 91330 (USA)
Supporting Information for this article is available on the WWW under
http://dx.doi.org/10.1002/cssc.201500848.
ChemSusChem 2015, 8, 3882 – 3891
collected from professional databases and the literature. The
results indicate that the perovskite dye is the primary source
of environmental impact, associated with 64.77 % total embod-
ied energy and 31.38 % embodied materials consumption, con-
tributing to more than 50 % of the life cycle impact in almost
all impact categories, although lead used in the perovskite dye
only contributes to about 1.14 % of the human toxicity poten-
tial. A comparison of perovskite solar cells with commercial sili-
con and cadmium–tellurium solar cells reveals that perovskite
solar cells could be a promising alternative technology for
future large-scale industrial applications.
this technology and its promising future in actual industrial-
scale applications, great concerns have been raised recently on
the potential environmental impacts of the perovskite solar
cell due to the heavy use of toxic chemicals, such as lead, and
energy-intensive processes, such as drying, heating up to
500 8C in the synthesis of perovskite dye, and solar cell manu-
facturing processes.[7] It has been widely recognized that more
than 70 % of a product’s environmental impact is determined
in the design and development stage,[8] and it is most effective
to conduct a comprehensive life cycle assessment (LCA) in the
early technology development stage to guide the sustainable
development of the technology.[9] Our rigorous literature
review only found two LCA studies related to solid-state perov-
skite solar cells published recently,[10, 11]but their environmental
impact results were significantly different from each other.
Gong et al. claimed that 82.5 and 60.1 g CO2 equiv could be re-
leased into the environment to generate 1 kWh of electricity,
with 7.78 kWh of manufacturing energy needed to fabricate
1 m2 TiO2 and ZnO solar cells.[10] Espinosa et al. found that
about 5.48 and 5.24 kg CO2 equiv were generated to produce
1 kWh of electricity, with 0.146 and 0.108 kWh of process
energy required to produce a 1 cm2 solar cell.[11] The are large
uncertainties with these two LCA results mainly because they
use secondary process data from the literature[10, 11] and ignore
supplementary materials, such as chemical solvents and associ-
ated energies needed for perovskite dye synthesis and the
solar cell fabrication process. No LCA study has been conduct-
ed on liquid perovskite solar cells. Although solid-state perov-
skite solar cells require more complicated manufacturing pro-
cesses and have a higher cost and environmental impact, this
3882 Ó 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

study presents an attributional LCA of liquid perovskite solar
cells to investigate their potential environmental impact from
cradle to gate and support sustainable scaleup in next stage of
research and development.
In perovskite solar cells, apart from the perovskite dye, the
electrode material and structure are also important in deter-
mining both the PCE performance and the environmental
impact of solar cell technology. Of various electrode materials
studied for high-performance perovskite solar cells, highly or-
dered TiO2 nanotubes (TNTs) demonstrate superior performan-
ces as photoelectrodes for solar cells compared with conven-
tional mesoporous TiO2.[12] The one-dimensional nanostructure
of TNTs can decouple the directions of light absorption and
charge-carrier collection,[13] which can provide more flexibility
for solar cell design. More importantly, the nanotube arrays
can significantly enhance light absorption with improved light-
trapping ability and increase the charge collection efficiency
with fast charge-transport channels. Additionally, the geometry
of the TNTs, such as pore size and tube length, can be con-
trolled precisely, which can help enormously in solar cell struc-
ture optimization and performance improvement.[14] Although
TNT-based perovskite solar cells have many advantages in
technology development, their environmental impact can be
significant due to the use of large amounts of organic chemi-
cals; high energy requirements for solar cell fabrication; and,
particularly, novel nanowaste emissions generated from the
process, which have never been investigated previously.
The objective of this study is to conduct a cradle-to-gate
LCA of liquid perovskite solar cell technology with TNT electro-
des to identify potential opportunities for improvement and
guide the sustainable development of liquid perovskite solar
cell technology from design to manufacturing. Herein, all man-
ufacturing process data are directly collected from our experi-
ments rather than those reported in the literature, which ena-
bles this study to be conducted at the process level with accu-
rate and reliable information to support the “design for sus-
tainability” of perovskite solar cell technology in the near
future. In addition, nanowastes and nanoemissions generated
from the TNT electrode manufacturing processes are character-
ized in an individual inventory, which could support future re-
search efforts in its environmental impact assessment and for
similar nanomanufacturing technologies. The following sec-
tions explain details of the experiments conducted in our lab,
LCA method, inventory, and impact analysis.
Experimental Section
TNT film-based anode manufacturing
Titanium foil was electrochemically anodized to give a titanium
nanotube film in mixed electrolyte in our laboratory; this is one of
the most commonly used manufacturing methods to produce
TNTs. Electrochemical anodization has great potential for industrial-
scale productions due to its easy, quick, and low-cost fabrication
process.[15] In our experiments, titanium foil (99.5 % purity, 0.25 mm
thick, Alfa Aesar) was ultrasonically washed with acetone for
15 min and rinsed with deionized water. A two-step anodization
was used to fabricate the well-ordered TNT film. The titanium foil
ChemSusChem 2015, 8, 3882 – 3891 www.chemsuschem.org
Full Papers
was first anodized in ethylene glycol (0.3 wt % NH4F and 0.6 vol %
H2O) by applying 70 V direct current (DC) potential for 2 h. The ob-
tained film was ultrasonically cleaned with deionized water to
remove the first oxidation layer. A second anodization process was
performed under 70 V DC potential for 5 min. The obtained TNT
film was annealed at 450 8C for 2 h and peeled off from the sub-
strate by an anodization-assisted self-detached approach.[16] For
solar cell anode fabrication, the fluorine-doped tin oxide (FTO)
glass was precoated with a titania blocking layer by spin-coating
a solution of 0.1 m titanium(IV) bis(ethyl acetoacetato)diisopropox-
ide in 1-butanol and heating at 500 8C for 30 min. Then, the free-
standing TNT film was transferred to FTO glass covered with titania
paste and annealed at 500 8C for another 30 min.[17] Detailed infor-
mation regarding anodization, titania paste, and FTO glass is given
in Sections 2 and 5 of the Supporting Information.
Perovskite dye preparation
The perovskite dye was synthesized by the reaction between
PbI2[18] and CH3NH3I. CH3NH3I was formed by the reaction of meth-
ylamine (23.5 mL, 40 % in methanol; TCI) and of hydroiodic acid
(30 mL, 57 wt % in water; Aldrich) in a 250 mL round-bottomed
flask at 0 8C for 2 h with stirring. The precipitate was recovered by
evaporation at 50 8C for 1 h. Then the product CH3NH3I was
washed with diethyl ether by stirring the solution for 30 min; this
was repeated three times. Finally, the product was dried naturally.
In this process, diethyl ether occupied about 84.05 % of the total
mass used to prepare the perovskite dye; this could be largely re-
duced by a recycling process in large-scale industrial productions.
To deposit perovskite dye onto the TNT-based anode, sequential
deposition methods were used.[19] Lead iodide was first introduced
into the TNTs by spin-coating (6500 rpm) a 462 mg mL¢1 solution
of PbI2 ( … 1 m) in N,N-dimethylformamide (DMF) for 5 s, followed
by heating at 70 8C for 30 min to dry PbI2. The TNT/PbI2 film was
then dipped into the prepared solution of CH3NH3I in 2-propanol
(30 mg mL¢1), rinsed with 2-propanol, and dried at 70 8C for 30 min.
In the reaction, the change of color from yellow to dark brown in-
dicated the formation of perovskite dye. The solution of 2-propa-
nol occupied 14.18 % of the total mass to prepare the perovskite
dye. Detailed information on energy and material consumption
can be found in Table 1. A complete GaBi model and LCI are illus-
trated in Section 4 of the Supporting Information.
The morphology of the TNT electrode before and after perovskite
dye deposition is presented in Figure 1. The cross-sectional image
of the nanotube arrays indicates a well-controlled nanotube struc-
ture obtained in the experiment (Figure 1 a). The inset of Figure 1 a
presents an overview of the structure of the TNT electrode with
a controlled thickness of 2.3 mm, which can provide a good PCE of
6.5 %.[12c] After deposition of the perovskite absorber, some nano-
Figure 1. Cross-sectional images of TNT before (a) and after (b) perovskite
dye deposition. The insets show a low magnification image of the film and
a TEM image of a single TNT/CH3NH3PbI3 deposition, respectively.
3883 Ó 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
 Full Papers
Platinum precursor-based cathode manufacturing
Table 1. LCI of materials and energy used to fabricate each subcompo-
nent per cm2. Platinum precursor paste (0.01 m H2PtCl6 in 2-propanol) was
dipped to the top edge of the FTO glass and heated to 450 8C for
Component Mass
15 min. The platinum precursor paste was comprised of chloropla-
[kg cm¢2] [%]
tinic acid and 2-propanol, which formed 0.52 and 99.48 % of the
perovskite dye total cathode materials, respectively. A detailed GaBi model and in-
CH3NH3I 1.59 Õ 10¢5 0.19 ventory for preparing the platinum precursor are shown in Fig-
2-propanol 4.17 Õ 10¢4 4.92
ure S8 and Table S14 in the Supporting Information.
diethyl ether 7.13 Õ 10¢3 84.05
PbI2 4.62 Õ 10¢5 0.54
DMF 8.79 Õ 10¢5 1.04
2-propanol for cleaning 7.86 Õ 10¢4 9.27
Electrolyte
energy consumption [kWh] 5.25 Õ 10¢3 The electrolyte was composed of 0.9 m LiI, 0.45 m I2, 0.5 m 4-tert-bu-
materials consumed 7.70 Õ 10¢3 100
tylpyridine (tBP), and 0.05 m urea in ethyl acetate, and no electricity
synthesized perovskite dye 6.20 Õ 10¢5
was consumed in this step. Ethyl acetate contributed 99.97 % of
TNT-based anode the total electrolyte in weight and the rest of the electrolyte com-
titania paste 7.89 Õ 10¢6 15.57 ponents formed only 0.03 % of the total mass. The full LCI of the
TNT film 1.65 Õ 10¢6 3.26 electrolyte is summarized in Table 1 and the GaBi model for LiI can
titanium(IV) bis(ethyl acetoacetato)diisopropoxide 2.12 Õ 10¢6 4.18 be found in Figure S9 and Table S15 in the Supporting Information.
1-butanol 3.90 Õ 10¢5 76.98
energy consumption [kWh] 2.59 Õ 10¢3
prepared anode 5.07 Õ 10¢5 100 Balance of system
TNT film Because the boundary of this research is from raw material extrac-
Ti foil 1.13 Õ 10¢4 0.49 tion to electricity generation, the system also included the materi-
acetone 8.00 Õ 10¢4 3.47 als and energy used to connect the PV module to the grid and
deionized water 2.06 Õ 10¢2 89.4 from the grid to the junction box of the building (balance of
ethylene glycol solution 1.53 Õ 10¢3 6.64
system, BOS). The mounting structure, inverter, and electric installa-
energy consumption [kWh] 3.22 Õ 10¢3
materials consumed 2.30 Õ 10¢2 100
tion were three main components of the BOS.
fabricated TNT film 1.65 Õ 10¢6 Herein, the TNT perovskite solar cell panel was assumed to be in-
stalled on a slanted roof; this is the most commonly used mount-
Pt precursor cathode
ing structure for solar cells. The selection of the inverter and elec-
Pt deposition 4.10 Õ 10¢7 0.52
2-propanol 7.85 Õ 10¢5 99.48
tric installation was based on the power generation and conver-
energy consumption [kWh] 6.47 Õ 10¢4 sion efficiency. Herein, electricity generation was presumed to be
prepared cathode 7.89 Õ 10¢5 100 3 kWp and the energy conversion efficiency was initially based on
the current laboratory-scale PCE (6.5 %) of the TNT perovskite solar
electrolyte cell with liquid electrolyte, but expanded to 25 % in the sensitivity
lithium iodide 1.20 Õ 10¢8 0.01 analysis, according to its theoretical maximum efficiency. A detailed
iodine 1.14 Õ 10¢8 0.01 inventory (Table S16 in the Supporting Information) was extracted
4-tert-butylpyridine 6.76 Õ 10¢9 0.01 from the Eco-invent database and Life Cycle Inventories of Photovol-
urea 3.00 Õ 10¢10 0
taics.[20]
ethyl acetate 8.97 Õ 10¢5 99.97
synthesized electrolyte 8.97 Õ 10¢5 100

FTO substrate Other materials for solar cell assembly

FTO glass for anode 1.25 Õ 10¢3 50.00
The counter electrode glass was drilled with two holes and con-
FTO glass for cathode 1.25 Õ 10¢3 50.00
FTO substrate 2.50 Õ 10¢3 100
nected to the positive electrode by a gasket. Then heat and pres-
sure were applied to the gasket (iron, 110 8C) for 60 s to connect
other materials for assembly the two electrodes. The two holes, which were used to fill the elec-
FTO glass 5.00 Õ 10¢6 75.36 trolyte, needed to be sealed by glass caps and gaskets. Applying
gasket 1.64 Õ 10¢6 24.64 heat and pressure (iron, 110 8C) for 20 s to the seals helped the
energy consumption [kWh] 1.08 Õ 10¢3 gasket to melt. The detailed inventory for sealing the holes on the
perovskite solar cell assembly 6.64 Õ 10¢6 100 substrates and connecting the two electrodes is shown in Table 1.
TNT-based perovskite solar cell [kg] 2.79 Õ 10¢3 Detailed mass and energy flows for the perovskite solar cell assem-
total energy consumed [kWh] 1.28 Õ 10¢2
bly are illustrated in Figures S1 and S2 in the Supporting Informa-
total materials consumed [kg] 3.34 Õ 10¢2
tion.

Life cycle assessment

particles attached to the wall of the nanotubes (Figure 1 b), and
the TEM image (inset of Figure 1 b) indicates successful infiltration
of the perovskite absorber into the nanotubes.
Life cycle assessment (LCA) is a systematic approach to evaluate
the comprehensive environmental impact of a product over its full
life cycle. A complete cradle-to-gate LCA of TNT perovskite solar
cells was conducted by including goal and scope definition, life
cycle inventory (LCI) analysis, life cycle impact assessment (LCIA),

ChemSusChem 2015, 8, 3882 – 3891 www.chemsuschem.org 3884 Ó 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

and interpretation. The inventory data was composed of energy
and material consumption. The energy demand in component
manufacturing was estimated as the product of equipment usage
time; power; and use factor, which was defined as the volume of
the manufacturing material divided by the maximum capacity pro-
duced by the equipment. The amount of materials used was calcu-
lated by multiplying the concentration (density) and volume. Other
LCI data, such as raw material extraction and part of material proc-
essing, were modeled and retrieved from the GaBi 6.0 professional
database, the EcoInvent database, and various reports in the litera-
ture. LCIA was conducted using standard impact categories and
characterization factors built into GaBi 6.0. Subsequently, sensitivity
analysis was carried out to investigate the effects of parameters
such as solar insolation, conversion efficiencies, and lifetime on the
environmental impact of TNT perovskite solar technology. Uncer-
tainty analysis was also performed to check the data quality and
robustness of the results. Finally, suggestions and recommenda-
tions were formulated according to the obtained impact results
and derived analysis.
Results and Discussion
Because perovskite solar cells are still under development and
have not entered the real application stage, in this study LCA
is applied to TNT-based perovskite solar cells with liquid elec-
trolyte to determine their environmental impact for the cradle-
to-gate life cycle phases, which excludes the usage and de-
commissioning phases. In the usage phase, a small amount of
water is used to clean the solar panel on an annual basis; this
is neglected herein.[20] For the decommissioning phase, there is
no industrial data for solar cell recycling and treatment be-
cause the life span of solar cells is as high as 30 years. Most
end-of-life research on solar cells is based on assumptions, and
perovskite solar cells, as third-generation solar cells, have no
valuable recycling data to input in our model.[21] However, for
perovskite solar cells, end-of-life is important due to the toxici-
ty of the perovskite dye, and future work will be conducted in
this area to optimize research. The cradle-to-gate life cycle of
TNT perovskite solar cells is divided into four main phases: raw
material extraction, material processing, component manufac-
turing, and TNT perovskite solar cell assembly (Figure 2). Raw
material extraction includes all processes that are used to ac-
Figure 2. System boundary of TNT film based perovskite solar cells.
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Full Papers
quire the raw materials. Notably, aggregated processes, such
as FTO glass manufacturing and isopropanol preparation in
the electrolyte, are also included in raw material extraction be-
cause they are not required to be further processed and their
products can be directly used in component manufacturing.
Material processing contains all procedures from raw materials
to the materials that can be directly used to fabricate the com-
ponents in the solar cells. Component manufacturing is the ex-
periments conducted in our laboratory to fabricate the solar
cell components, including perovskite dye, TNT film based
anode, platinum precursor cathode, electrolyte, FTO substrates,
other materials for assembly, and the balance of system (BOS).
The total mass of TNT perovskite solar cell is composed of
2.22 % perovskite dye, 1.82 % TNT anode, 2.83 % Pt precursor
cathode, 3.22 % electrolyte, 89.61 % FTO glass, and 0.24 %
other materials for assembly. For a comparative analysis with
other solar cell technologies, the impact of transportation in
this LCA study is neglected by assuming that perovskite solar
cells have a similar impact from transportation as other solar
cell technologies. The functional unit in this study is defined as
1 cm2 active area for solar electricity generation, and it is inter-
changeable with other functional units, such as kWh under
specific solar insolation, performance ratio, and conversion effi-
ciency. Herein, the active area is defined as the area of TNT
film divided by the area of FTO glass, and is assumed to be
60 %.[22] Electricity consumption is based on the energetic mix
of the USA, in which hard coal (40.86 %), natural gas (24.04 %),
and nuclear power (18.89 %) are the major resources for
energy generation.
Life cycle inventory analysis
Materials and energy inventories are summarized in Table 1
and the LCI analysis of TNT perovskite solar cells is based on
the scope and boundaries defined above. The LCI analysis is
conducted by using a process-based LCA method; detailed
analyses can be seen in the following paragraphs.
The energy consumed in the life cycle of TNT perovskite
solar cells from cradle to gate is a major part of environmental
impact analysis. Energy is consumed from raw material extrac-
tion to electricity generation,
and the total embodied energy
is calculated to be 0.27 kWh to
produce a 1 cm2 active area TNT
perovskite solar cell (2.79 g). The
manufacturing energy used in
the process to fabricate the solar
cell is calculated to be
0.01 kWh cm¢2, which is compa-
rable with traditional dye-sensi-
tized solar cells (DSSCs) reported
in the literature.[23] Major embod-
ied energy-intensive processes
are preparation of the perovskite
dye (0.178 kWh cm¢2) and TNT-
based anode (0.074 kWh cm¢2).
Notably, TNT film fabrication is
3885 Ó 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

the major energy-consumption source for anode fabrication
(0.060 kWh cm¢2). It is also worth noting that the preparation
of perovskite dye is the most energy-consuming procedure of
all energy-intensive processes; this mainly originates from the
consumption of diethyl ether, 2-propanol, and synthesis
power. Specifically, about 10 mL of diethyl ether is needed to
wash the CH3NH3I precipitate and the extraction of diethyl
ether uses 0.120 kWh of energy. The production of 2-propanol
consumes about 0.028 kWh of energy. The power used in
spin-coating, evaporating, and cleaning requires approxi-
mately 0.025 kWh per cm2 of active area. On the other hand,
TNT film fabrication is another energy-intensive process, which
results from the use of a large amount of etching (ethylene
glycol) and cleaning (acetone) solutions, which consumes
0.033 kWh of energy altogether. Meanwhile, 0.016 kWh of
power is used in anodization, which involves electricity usage,
such as a DC power supply and a heating oven. A detailed
energy flow diagram is shown in Figure S2 in the Supporting
Information.
Material consumption in fabricating TNT perovskite solar
cells is another major part of the life cycle environmental
impact. As calculated, a total of 8.58 kg of materials are used
in raw material acquisition from cradle to gate to produce
a 1 cm2 active area TNT perovskite solar cell. Major material-
consuming processes are preparation of the TNT film based
anode (5.04 kg cm¢2) and perovskite dye (2.69 kg cm¢2), which
take about 90 % of the total material consumption. Through
calculations, the high material consumption is associated with
electricity generation and solvent preparation. The result also
indicates that the TNT anode consumes more materials than
perovskite dye preparation; this may originate from the large
amount of raw materials used to produce the TNT etching so-
lution. Specifically, ethylene glycol and acetone are two materi-
al-intensive solvents used in TNT-based anode manufacturing,
with 1170 and 585 kg total materials needed to prepare 1 kg
of ethylene glycol and 1 kg of acetone, respectively. However,
for perovskite dye preparation, the most material-consuming
solvent is diethyl ether, which requires 35.8 kg of raw materials
for 1 kg of substance. The material composition of the TNT
perovskite solar cell is summarized in Table 1. A detailed mass
flow is modeled in GaBi 6.0 and shown in the Figure S1 in the
Supporting Information.
Nanowastes and nanoparticle emissions generated from TNT
film fabrication are also important sources of environmental
impact that should be considered in the LCA study.[9] However,
the environmental fate, transport, and toxicity models required
for environmental impact assessments of nanoparticles are still
under development. Commercially available LCA databases,
such as GaBi, do not include the environmental impact of
nanowastes and emissions. Previous reports have identified
that the environmental impacts of nanowastes and emissions
are highly dependent on the particle shape, size, mass, surface
charge, and among others.[24] Herein, these relevant parame-
ters of nanowastes and emissions are characterized and ana-
lyzed in a separate inventory (Figure 3) to provide information
to further develop environmental impact assessment methods
for these nanowastes and nanoemissions.
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Figure 3. Nanowastes from TNT film fabrication: a) low- and b) high-resolu-
tion SEM images of TNT waste on FTO glass, c) energy-dispersive X-ray spec-
troscopy (EDS) spectrum of Ti and O waste [content: 58.2 wt % (30.7 at %) Ti;
35.3 wt % (55.7 at %) O; 6.5 wt % (13.6 at %)] and d) nanoparticle size distribu-
tion.
The solid nanowastes from TNT electrode fabrication are an-
alyzed. Figure 3 a and b show low- and high-magnification
SEM images, which indicate that the wastes are mainly com-
posed of broken TNTs. EDS characterization (Figure 3 c) con-
firms the composition of the solid wastes, in which the Ti and
O peaks are derived from TiO2, and the C peak is from the
carbon paste of the sample stage. Quantitative analysis of the
EDS spectrum gives a Ti/O atomic ratio of about 1:2 (Figure 3 c,
inset). Figure 3 d shows results from the zeta-potential analysis
of the nanoparticle size and distribution of the solid waste,
with a mean diameter of 5626.4 nm and geometric standard
deviation of 1.885. Additional nanoparticle emission data from
the TNT synthesis is listed in Figure S10 in the Supporting In-
formation.
Life cycle impact assessment
The environmental impact of TNT perovskite solar cells from
the cradle to the gate have been calculated and characterized
by means of the ILCD (International Reference Life Cycle Data
System) method in GaBi 6.0 (Figure 4). The LCIA of different
components are expressed as patterned bars in Figure 4,
whereas the environmental impact from four different life
cycle stages are shown as colored bars, which include raw ma-
terial extraction, material processing, component manufactur-
ing, and perovskite solar cell assembly. Notably, nanowastes
and nanoemissions are not included in the impact assessment
because there are no characterization factors or metrics avail-
able in current LCIA methods to perform the analysis.
The process-based LCIA shows that most of environmental
impact is generated from raw material extraction, and this can
be explained by large amounts of energy and materials used
to extract solvents used in perovskite solar cell manufacturing.
During synthesis of the perovskite dye, the solvents used to
clean and dissolve the chemicals, as measured in our experi-
ments, occupy about 50 % of the total mass. As a result,
perovskite dye synthesis forms the major portion of the envi-
Ó 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Figure 4. Life cycle environmental impact of TNT film based perovskite solar
cells from the cradle to the gate: acidification potential (AP), freshwater eco-
toxicity potential (ETP), eutrophication potential (freshwater EP), human tox-
icity potential (HTP), ionizing radiation (IR), global warming potential (GWP),
ozone depletion potential (ODP), respiratory inorganics (RI), photochemical
ozone creating potential (POCP), and abiotic depletion potential (ADP).
ronmental impact, contributing to 43.54 % AP, 79.42 % ETP,
91.14 % EP, 59.59 % HTP, 74.00 % IR, 53.31 % GWP, 81.29 % ODP,
53.58 % RI, 55.33 % POCP, and 69.54 % ADP, and is associated
with 64.77 % total embodied energy and 31.38 % materials.
The high EP and ODP percentages are mainly due to the large
amounts of diethyl ether, 2-proponal, and other organic sol-
vents used in perovskite dye synthesis. From Figure 4, it can
also be seen that TNT film fabrication has a higher environ-
mental impact than the other components, except perovskite
dye, in most of the categories, such as AP, HTP, and GWP. Simi-
larly, it is also caused by the large amounts of organic solvents
used to clean and dissolve the chemicals in TNT film fabrica-
tion, which suggests that more attention should be paid to re-
ducing the use of solvents for the sustainable development of
perovskite solar cells in future mass-production scales.
Among different life cycle stages, raw material extraction,
which is mainly related to solvent usage, is the process with
the highest environmental impact, and contributes to more
than half of the life cycle impact in most categories (Figure 4),
such as AP (75.47 %), ETP (90.04 %), EP (98.25 %), HTP (47.49 %),
IR (95.65 %), GWP (69.18 %), ODP (98.30 %), RI (72.79 %), POCP
(88.16 %), and ADP (54.20 %). The high environmental impact
percentage in each category is mainly due to high energy and
material consumption. Raw material extraction takes up
77.06 % of the total energy and 35.09 % of total material con-
sumption. Notably, the solvents utilized in TNT film fabrication
and perovskite dye preparation share 66.08 % total energy and
31.07 % total mass, which confirms that the use of solvents is
the most significant source of life cycle emissions. Therefore,
the most effective way to reduce the environmental impact of
TNT-based perovskite solar cells is to recycle and reuse sol-
vents from perovskite solar cell manufacturing.
Apart from solvent consumption, manufacturing energy is
another noteworthy factor that drives the overall environmen-
ChemSusChem 2015, 8, 3882 – 3891 www.chemsuschem.org
Full Papers
tal impact. The manufacturing energy contributes to 23.60 %
AP, 0.59 % ETP, 0.039 % EP, 50.06 % HTP, 1.84 % IR, 30.24 % GWP,
0.56 % ODP, 25.86 % RI, 11.19 % POCP, and 43.87 % ADP. Higher
AP, HTP, GWP, and ADP values mainly originate from hard coal
burning activities, which accounts for 40.86 % of the electricity
mix in the USA, but has the lowest heating value and efficiency
compared with those of heavy fuel oil and natural gas.[25] Of all
component manufacturing processes, TNT film based anode
manufacturing and perovskite dye preparation contribute
most to process energy. TNT film based anode manufacturing
involves several processes that have a high energy demand, in-
cluding anodization with a DC power supply and multiple
high-temperature calcination processes. For perovskite dye
preparation, a large amount of energy is used to evaporate
precipitated CH3NH3I and to dry the coated PbI2 crystal and
perovskite dye in the oven. Therefore, developing a low-tem-
perature approach for perovskite dye and TNT anode prepara-
tion should be an efficient way to decrease energy consump-
tion, and consequently, reduce the environmental impact.
Because the use of lead in perovskite dye is a major concern
due to the material’s high toxicity,[7] the human toxic cancer
effect has been employed herein to analyze the effects of lead
in the TNT perovskite solar cell production process, which has
the second largest normalized value of all environmental
impact factors and indicates that the fabrication of perovskite
solar cells has a relatively high HTP intensity in the USA (nor-
malized environmental impact factors can be found in
Table S21 in the Supporting Information). Surprisingly, process
energy and solvent usage are two major factors that affect the
human toxic cancer effect, rather than lead used in perovskite
dye preparation. On one hand, the high HTP values of process
energy and solvent production are mainly due to the large
amounts of material and energy consumption, as stated previ-
ously. The production of solvents takes about 66.06 % of the
total energy and 31.07 % of the total materials. Moreover, the
process energy occupies 22.55 % of the total energy and
64.67 % of the total mass. On the other hand, the production
of lead nitrate, which has greater energy and material con-
sumption than that of lead, only depletes 0.25 % of the total
energy and 0.75 % of the total materials. Consequently, the
lower HTP value of lead is the result of the smaller portion of
energy and material consumption. Emissions generated from
the energy and solvent production processes also contribute
to the high HTP value. According to the GaBi database, both
energy and solvent production processes will generate a certain
amount of gaseous emissions, including SO2, NOx, CO, non-
methane volatile organic compounds (NMVOCs), and particu-
late matters (PM10 and PM2.5), which have relatively high
HTPs. Meanwhile, metals, such as iron, magnesium, and alumi-
num, emitted into the water system are another noteworthy
part of the high HTP value in both production processes. The
combined manufacturing energy for solar cell components
takes up 50.06 % of the HTP, which indicates that electricity
usage has a great impact on the toxicity potential. Meanwhile,
diethyl ether is still a significant impact factor with an HTP
value of 29.35 %. As a result, more attention should be concen-
trated on the reduction of process energy and solvent usage
3887 Ó 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

in developing perovskite solar cells. It is also well known that
industrial-scale production can largely increase the electricity
usage efficiency, and hence, greatly reduce energy consump-
tion. An estimation of the environmental impact changes
under scaled-up production is further executed in GaBi. As il-
lustrated in Table S20 in the Supporting Information, with
a 20 % manufacturing energy reduction, a decrease of 4.2 %
GWP and 9.7 % HTP can be obtained.
To clarify the major process that has high HTP during perov-
skite dye preparation, the synthetic process for the perovskite
dye itself is analyzed separately during the cradle-to-gate life
cycle. CH3NH3I is responsible for 62.31 % HTP because of high
material consumption and the large characterization factors in
solvent and process energy production. In comparison, lead
iodide is only responsible for 3.68 % HTP, with 7.93 % of the
total material consumed during its synthesis. Notably, the pro-
duction of lead itself contributes less than 0.37 % HTP in the
perovskite dye preparation process due to the small amount
of lead involved in the process. To produce the 1 cm2 active
area TNT-based perovskite solar cell, only 0.046 g of PbI2 (0.1 m,
2 drops of PbI2 in DMF) is needed. Contrary to our expecta-
tions, the process to produce CH3NH3I has a much higher HTP
than that of the procedure to synthesize PbI2. The use of dieth-
yl ether and 2-propanol in CH3NH3I preparation is responsible
for the high impact on the human toxic cancer effect. The re-
sults indicate that CH3NH3I, rather than the lead in perovskite,
should be the major concern for the perovskite sustainability
performance during the manufacturing process.
Overall, the most significant environmental impact factor is
solvent usage, and therefore, solvent reclamation could be the
most promising way to reduce the total environmental impact.
It has been proven that recycled solvents can be reused in
semiconductor manufacturing to serve as solvents for organic
synthesis.[26] The purity of the recycled solvent is highly depen-
dent on the properties of each solvent and can reach 99.5 % or
higher,[27] which should meet the quality requirements for solar
cell production in most cases. Moreover, the energy usage and
material consumption for recycling could be much lower than
solvent production. Based on the recycling model built into
GaBi, only 1.64 kWh of energy is needed in the recycling pro-
cess to regenerate 1 kg of solvent. However, producing 1 kg of
organic solvent will cost much more energy, ranging from 9.7
to 16.2 kWh. For instance, about 12.4 kWh of energy is needed
to produce 1 kg of diethyl ether. To estimate the effects of sol-
vent renewal, the scenario with solvent recycling is modeled in
GaBi 6.0. It turns out that, with an average recycling rate of
86 % in industry,[27a, 28] most environmental impact is reduced
significantly. For instance, ETP, EP, and IR are reduced by 62.6,
74.3, and 49.4 % respectively; GWP also decreases from 28.8 to
23.5 g CO2 equiv. The results of life cycle environmental impact
reduction from solvent recycling are shown in Table S19 in the
Supporting Information, and reduced life cycle environmental
impact from recycling solvents in each perovskite component
and in each LCA phase are illustrated in Figures S13 and S14 in
the Supporting Information, respectively.
ChemSusChem 2015, 8, 3882 – 3891 www.chemsuschem.org 3888
Full Papers
Sensitivity and uncertainty analysis
Sensitivity analysis is performed by evaluating the life cycle
emissions to generate 1 kWh of electricity. Power generation
can be estimated by G = E Õ I Õ PR Õ L Õ A,[29] in which G, E, I, PR,
L, and A represent the power generated, conversion efficiency,
insolation, performance ratio, lifetime, and active area, respec-
tively. In the calculation, A is 60 % according to the scaled-up
production[22] and PR is 0.75 in Europe and 0.95 in the USA,
which represents that about 25 or 5 % of energy is lost due to
the BOS and other indirect processes.[23b, 30] Other factors that
affect the power generation of TNT perovskite solar cells, in-
cluding E, I, and L, are defined as the sensitivity parameters in
our analysis (Table S22 in the Supporting Information). It is as-
sumed that module efficiency and lifetime can be increased
without large fluctuations of energy and material consumption
in this study. According to current research, the increase in
perovskite solar cell efficiency strongly depends on the im-
proved quality of the deposited perovskite crystal, which is
mainly achieved by optimizing the spin-coating process.[31] This
process has relatively low material and energy consumption,
and therefore, may only cause small fluctuations on the envi-
ronmental impact. For instance, the manufacturing energy is
concentrated on the preparation of perovskite dye, which con-
sumes about 48.65 % of the total manufacturing energy. From
this amount of energy, about 97.7 % of the energy is used by
evaporation when synthesizing CH3NH3I, and cannot be avoid-
ed by most CH3NH3PbI3 synthetic approaches. Therefore, it is
reasonable to assume a relatively stable process energy for
perovskite dye development. Notably, possible differences
caused by perovskite solar cell structural evolution are neglect-
ed due to a lack of industry production data at this early devel-
opmental stage. With these hypotheses, different insolation,
conversion efficiencies and lifespans have been considered in
the sensitivity analysis to evaluate changes to the environmen-
tal impact. The results for different environmental categories
are illustrated in Figure 5 and Table S23 in the Supporting In-
formation, and show that the life cycle emissions from differ-
ent categories are highly dependent on the sensitivity parame-
ters. Specifically, the environmental impact from the ten cate-
gories is linearly correlated with sensitivity factors. Taking GWP
as an example, GWP is inversely proportional to solar insola-
tion, conversion efficiency, and lifetime (Figure S15 in the Sup-
porting Information). If the insolation changes from 1000 to
2190 kWh m¢2 per year in Europe under fixed conversion effi-
ciency (6.5 %), lifetime (5 years, based on the commercial solar
cell), and performance ratio (0.75), the GWP will vary from
1173.3 to 535.8 g CO2 equiv to produce 1 kWh of electricity.
Meanwhile, if the insolation varies from 1359 to 2143 kWh m¢2
per year in the USA under 6.5 % conversion efficiency, with
a fixed lifetime of 5 years and 0.95 performance ratio, the GWP
will change from 681.6 to 432.3 g CO2 equiv. Moreover, with
a fixed insolation and lifetime, GWP will decrease linearly with
increasing PCE. For a solar panel installed in the USA with
1860 kWh m¢2 per year insolation and a fixed lifetime of
5 years, the GWP will decrease from 497.2 to 129.3 g CO2 equiv
if the conversion efficiency increases from 6.5 to 25 %. Also,
Ó 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Figure 5. Sensitivity analysis of environmental impact: a) sensitivity analysis with changes to insolation (conversion efficiency of 6.5 %; lifetime of 5 years; at
1000, 1700, and 2190 kWh m¢2 per year the PR is 0.75; at 1359, 1860, and 2190 kWh m¢2 per year the PR is 0.95); b) sensitivity analysis with change to conver-
sion efficiency (insolation of 1860 kWh m¢2 per year; lifetime of 5 years; PR of 0.95); c) sensitivity analysis with changes to lifetime (1, 5, 15, and 30 years). *uni-
fied factors: GWP, ETP, EP Õ 104, IR Õ 0.1, ODP Õ 108, RI Õ 104, ADP Õ 105, HTP Õ 108, POCP Õ 103, AP Õ 103.
with increasing lifetime from 1 to 30 years, the GWP reduces
from 2486.1 to 82.9 g CO2 equiv under 1860 kWh m¢2 per year
insolation and 6.5 % conversion efficiency. Because power gen-
eration is the multiplication of different sensitivity parameters,
they have the same impact on the final results. The increase of
any one of the sensitivity parameters can equally enhance
electricity generation and decrease greenhouse gas (GHG)
emissions. The results suggest that the environmental impact
can be effectively reduced by an overall improvement in the
conversion efficiency, longevity, active area ratio, and per-
formance ratio.
Because perovskite solar cells are still in the early stages of
research and development, and the manufacturing process pa-
rameters for large-scale production have not been fully estab-
lished yet, the LCA based on the laboratory-scale experiments
will have some uncertainties in the LCA results. Three major
uncertainty sources are identified and considered in this analy-
sis. The first one is methodological uncertainty. Herein, method
uncertainty is mainly associated with concerns about calculat-
ing the HTP impact category. Currently, toxicity assessment is
a challenge in LCA studies because a robust model for charac-
terization factor development is lacking.[32] In this study, the
HTP category is characterized according to the USEtox
method, which is a widely accepted model in current LCA
practices. However, the uncertainty range of HTP is still consid-
erable and gives two to three orders of magnitude factors for
characterization factors on human health.[33] Thus, the impact
value from the HTP category should be treated with caution,
particularly when comparing two different products.
The second source of uncertainty is induced by the variabili-
ty of input parameters that cause variations of environmental
impact in the end product. Monte-Carlo analysis is employed
herein to assess the cumulative effect of uncertainties from dif-
ferent inputs. In this study, the uncertainty of GWP is analyzed
by changing material and energy inputs by œ 10 and œ 20 %.
The list of changing data is shown in Table S24 in the Support-
ing Information. The probability density of equivalent CO2
emissions has been plotted in Matlab and is illustrated in Fig-
ure S17 in the Supporting Information. The mean value of
CO2 equiv emissions is 28.8 g. The detailed Monte-Carlo analy-
sis can be found in Section 13 in the Supporting Information
ChemSusChem 2015, 8, 3882 – 3891 www.chemsuschem.org
Full Papers
and the results show that the standard deviation is 3.6 and
7.12 g with a 95 % confidence interval, which indicates that the
final results are reliable with œ 10 and œ 20 % changes to
energy and material consumptions.
The last source of uncertainty originates from the lack of
impact assessment for nanowastes and nanoparticle emissions
generated from the TNT film fabrication process. This uncer-
tainty will add additional values to the life cycle impact catego-
ry, especially RI and toxicity potentials, because both of them
have been demonstrated to be closely correlated with the
emissions of fine metal particles. With progress of research
into nanotoxicity and impact assessment methods, this uncer-
tainty could be addressed in the near future with the com-
munity’s joint efforts in this direction.
Benchmarking with other solar cells
To evaluate the sustainability potential of perovskite solar cells
on the future market, the life cycle environmental impact of
the perovskite solar cells is benchmarked with Si solar cells,
thin-film CdTe solar cells, and DSSCs (Table 2 and Table S25 in
the Supporting Information). The comparison is based on avail-
able common impact data in manufacturing energy; GHG
emissions; and energy payback time (EPBT), which is defined
as the time required for a renewable energy system to gener-
ate the same amount of energy as that used to produce the
system itself. Current results indicate that the manufacturing
energy used in the TNT perovskite solar cell is much smaller
than that in silicon solar cells and CdTe solar cells, but similar
to that of traditional DSSCs and larger than that of solid-state
DSSCs. Additionally, from the results shown in Table 2, the
GHG emissions and EPBT values for perovskite solar cells based
on current laboratory-scale data have a wider range than that
of traditional solar cells. Considering future large-scale applica-
tions and the rapid development of perovskite solar cell tech-
nology, which could significantly reduce energy consumption
of the process and improve the PCE, GHG, and EPBT values,
perovskite solar cell technology could become comparable to
commercial Si and CdTe solar cells. Moreover, it is also noted
that our data has a larger maximum bound than other perov-
skite solar cells,[34] and this can be explained by the large
3889 Ó 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Table 2. Benchmarking of LCA results with other solar cells.
Types of solar cell Manufacturing GHG emissions[b]
energy[a] [kWh] [g CO2 equiv]
mono-Si[35] 794–1459 29–45
multi-Si[35] 750–1431 23–44
a-Si[35] 197–553 18–50
Cd-Te[35] 219–501 14–35
DSSCs[23a, b, 36] 12–280 19–120
solid-state perovskite[10, 11] 7.78 60.1–5480
TNT film-based perovskite 128 18.7–5867
[a] Per cm2. [b] To produce 1 kWh electricity.
amount of solvent considered in this analysis, which is usually
neglected or underestimated in other studies.[34] The bench-
marking results indicate that the TNT perovskite solar cell is
a sustainable solar technology with competitive environmental
benefits of moving toward future industrial-scale applications.
Conclusions
Perovskite solar cells have attracted enormous attention as
a promising solar technology due to their low cost and superi-
or conversion efficiency. However, the use of toxic metals, such
as lead, in the perovskite dye and chemicals such as diethyl
ether and other organic solvents in manufacturing has caused
significant concerns for their potential environmental impact.
To facilitate the sustainable development of perovskite solar
cell technology, herein, a cradle-to-gate life cycle environmen-
tal impact study of TNT-based perovskite solar cells is per-
formed by using an attributional LCA approach, with both pro-
cess-based laboratory-scale manufacturing data and literature-
based upstream data from GaBi 6.0 professional and Ecoinvent
databases employed for the environmental impact assessment.
Our results that the most significant environmental impact
factor is the solvent used in perovskite dye synthesis and TNT
anodization, and the second most important is the energy con-
sumption of the process. The contribution from lead is surpris-
ingly low due to its very small amount of usage, as confirmed
by the human toxic cancer effect assessment by using the HTP
metric. The LCA results suggest that solvent reclamation or re-
duction and energy-efficient manufacturing processes are es-
sential for sustainable development of perovskite solar cell
manufacturing. Compared with commercial silicon and cadmi-
um–tellurium solar cells, perovskite solar cells present a much
smaller manufacturing energy consumption and comparable
GHG emissions and EPBTs. Perovskite solar cells will have
a promising future in replacing silicon and cadmium–tellurium
solar cells in future commercial markets.
Keywords: life cycle assessment · dyes/pigments ·
photochemistry · renewable resources · sustainable chemistry
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ChemSusChem 2015, 8, 3882 – 3891 www.chemsuschem.org 3891 Ó 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim