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Economic and LCA of Recycling EoL Silicon PV Modules (Lim - 2022)
Economic and LCA of Recycling EoL Silicon PV Modules (Lim - 2022)
Economic and LCA of Recycling EoL Silicon PV Modules (Lim - 2022)
A R T I C L E I N F O A B S T R A C T
Handling Editor: Mingzhou Jin The utilization of solar technology for clean energy generation has seen a dramatic increase over the past decade.
Eyeing the ever-growing solar capacity and the subsequent inevitable deluge of solar panel wastes, the ideal
Keywords: approach to handle End-of-Life (EoL) solar photovoltaic (PV) panels is to recycle their materials for reuse. This
Life cycle assessment (LCA) present study explores an optimal recycling process with a high resource recovery efficiency on a laboratory
Renewable energy
scale, which comprises of three main steps: module delamination, acid etching and sequential electrodeposition.
Solar energy
High recoveries of 86, 95 and 97% were achieved for silver, lead and aluminum, respectively. The acquired
Recycling
Economic analysis results are further applied in a life cycle assessment. The process was scaled up to simulate an industrial process
Silicon photovoltaic (PV) and its human and environmental impacts were compared to those of the landfilling disposal method, with six
main impact categories analyzed and described: global warming potential, human toxicity potential, freshwater
ecotoxicity potential, acidification potential, eutrophication potential and ozone depletion potential. Mitigation
strategies are also proposed. Lastly, economic analysis demonstrated that at a treatment capacity of 892.5 kg/h,
the process is feasible with an internal revenue rate of 28.2% and a payback time of less than a year, provided the
waste collection is subsidized.
* Corresponding author.
** Corresponding author.
E-mail addresses: gtpan@ntut.edu.tw (G.-T. Pan), faye1004@gmail.com (S. Chong).
https://doi.org/10.1016/j.jclepro.2022.130796
Received 9 September 2021; Received in revised form 28 December 2021; Accepted 30 January 2022
Available online 2 February 2022
0959-6526/© 2022 Elsevier Ltd. All rights reserved.
M.S.W. Lim et al. Journal of Cleaner Production 340 (2022) 130796
Fig. 1. Estimation of cumulative global waste (million tonnes) from End-of-Life solar PV panels (IRENA andIEA-PVPS, 2016).
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M.S.W. Lim et al. Journal of Cleaner Production 340 (2022) 130796
recover Ag and Si from EoL solar PV cells. In their study, over 99% purity
of both elements can be achieved. On the other hand, Luo et al. (2021)
performed a hydrometallurgical study to recover Al, Ag and Si from EoL
solar PV cells, with recovery efficiencies of 99.89, 96.13 and 96.03%. In
most recent studies (Ansanelli et al., 2021; Chen et al., 2020; Chung
et al., 2021; Daljit Singh et al., 2021; Dias et al., 2021; Mulazzani et al.,
2021; Riech et al., 2021; Wongnaree et al., 2020), economic analysis and
life cycle assessment were not included, limiting the environmental,
technical, economical and scalability prospects of the technique. It is
also noted that environmentally hazardous chemicals such as hydro
fluoric acid were used in the study, which presents a disadvantage from
an environmental point-of-view. Such cost analysis and environmental
evaluation results are significant drivers to facilitate the implementation
of effective and efficient recovery and recycling processes to avert
environmental disasters as a result of massive EoL solar panel wastes.
The huge market share of crystalline silicon based solar panels de Fig. 3. The research elements.
mands the invention and innovation of more diverse recovery and
recycling technologies in order to curb with the associated wastes,
2.1. Experimental
which are increasing at an alarming pace and henceforth serves as the
principal motive of this present study, as well as to connect with the cost
2.1.1. Disassembly and characterizations
and environmental studies as mentioned in the previous paragraph. This
A piece of EoL monocrystalline silicon solar PV panel with the di
study attempts to explore an efficient recycling process of EoL solar PV
mensions: 400 mm (length) × 200 mm (width) was provided by an
panels using HNO3, H2SO4 and H2O2 as the etching solvent to leach out
electronic waste recycling company. The solar panel was thoroughly
target resources such as Ag, Pb and Al, followed by electrodeposition to
cleaned with deionized water and weighed before manual disassembly.
recover the aforementioned resources, as well as the monocrystalline
Table 1 shows the components after the cleaning and before thermal
solar-grade silicon wafer. It is highlighted that electrodeposition has the
treatments. The solar cell piece was then thermally treated in an oven at
potential to be a more cost-efficient approach than other techniques
600 ◦ C for 1 h to remove the EVA layer.
such as precipitation in recovering the leached metals as it enables the
X-ray diffraction (XRD, PANalytical X’Pert PRO, Almelo, the
simultaneous recovery of multiple metals in their pure metallic forms
Netherlands) was used to verify the type of waste panel sample via its
from the leaching solution. Furthermore, a life cycle assessment is also
crystalline structure, with Cu K–alpha radiation (λ = 0.15418 nm)
performed on the recycling process and compared the landfill disposal
scanning from 20 to 90◦ . Field-emission scanning electron microscopy
method to determine their corresponding environmental impacts, with
(FE-SEM) with energy-dispersive X-ray spectroscopy (EDX) (JEOL JSM-
categories such as global warming potential (GWP), freshwater eco
6700F, USA) was used to obtain high-resolution images of the surface
toxicity potential (FEP), ozone depletion potential (ODP), human
morphology at an accelerating voltage of 10–12 kV and a working dis
toxicity potential (HTP), eutrophication potential (EP) and acidification
tance of 10–12 mm, with a magnification of 100–1000✕ in an envi
potential (AP). The analysis is carried out based on scaling up the pilot
ronmental mode. The characterization test was also used to carry out
scale process to a simulated industrial scale, in which appropriate
both elemental identification and to acquire quantitative compositional
treatment/disposal methods are proposed to minimize environmental
information of the samples.
impacts.
Furthermore, SuperPro Designer is used to simulate the recycling
2.1.2. Acid etching
process in this current study to enable the quantification of the economic
An acid etching method was used to leach out the target metals from
and environmental benefits obtained from the recovery and recycling of
the EoL solar cell. A mixed solution consisting of 10 mL nitric acid (69%
EoL solar panels as secondary raw materials for further usage. The
HNO3, Sigma-Aldrich) or 10 mL sulfuric acid (diluted to 50% from 98%
technical and economic feasibility of this recycling process including the
H2SO4, Sigma-Aldrich), 20 mL hydrogen peroxide (30% H2O2, ChemAR)
recovery of useful resources was simulated based on preliminary data
and 1 L deionized water was used as the etching solvent. H2O2 was
obtained from laboratory-scale research presented in this paper. The
added as a catalyst to speed up the leaching process. An ultrasonic
process simulations are described and analyzed to present an economic
shaker, placed in a fume hood, was filled with the etching solvent and
assessment of the recovery process.
the EoL solar cell was placed into the ultrasonic shaker for 10 min. In
In this paper, the characterization of the EoL solar PV cells is first
order to neutralize the leaching solution produced, 15.751 g of solid
described to determine and confirm their properties. Next, results from
sodium hydroxide (NaOH, 97%, Sigma-Aldrich) was added to the
the acid etching treatment of the EoL cells are described and analyzed.
leaching solution until a pH value close to 6 was attained. During this
Following, the recovery efficiencies of the useful resources from the PV
wastes are determined through constant-voltage electrodeposition and
precipitation. Lastly, LCA and economic feasibility analyses are per Table 1
formed to assess and ascertain the overall environmental, technical and Disassembled components of the EoL monocrystalline silicon solar PV panel
economic viability of this EoL solar PV recycling initiative. sample.
Components Mass (g)
2. Methodology 1 Junction box 12.329
2 Aluminum frame 172.230
Fig. 3 outlines the methodology of this study, starting with the 3 Glass layer 589.130
experimental evaluation – manual disassembly and characterizations, 4 Solar cell 31.212
5 EVA material 22.900
acid etching, and electrodeposition, followed by life cycle and economic 6 Plastic back sheet 23.450
assessments to evaluate the environmental impacts and economic 7 Copper cable 2.945
analysis of the process, respectively. 8 Screws 32.142
9 Others 6.162
Total weight: 886.338
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M.S.W. Lim et al. Journal of Cleaner Production 340 (2022) 130796
process, the presence of precipitation indicates that the aluminum ions Ci, 0 − Ci, Vi
were reacting with the hydroxide ions to form aluminum hydroxide, Recovery efficiency for other metals, Rm,i (%) = × 100% (2)
Ci, 0
which was then collected by filtration and dried at 105 ◦ C overnight to
recover the aluminum leached. ∑
RAl Ci, 0 + Rm,i Ci, 0
Overall recovery efficiency, R (%) = × 100% (3)
CT, 0
2.1.3. Cyclic voltammetry (CV) and electrodeposition
A ZIVE electrochemical workstation (ZIVE SP1, Wuhan Corrtest In where:
struments Corp., Ltd., Wuhan, China) was used to conduct the cyclic
voltammetry (CV) test and to carry out electrodeposition for the Ci,0 = Concentration of element i in leaching solution;
neutralized leaching solution. In the CV test, the reduction potentials Ci,0 = Concentration of element i in neutralized leaching solution;
required for the recovery of different metal elements were obtained by
Ci,Vi = Concentration of element i in leaching solution after electro
observing the redox peaks under the potential-dynamic condition from
deposition at the cell potential Vi obtained from CV;
− 2.5 to 2.5 V.
CT,0 = Total concentration of all recoverable metal elements in
For the electrodeposition of target metals, carbon fiber was used as
leaching solution.
the working and counter electrodes with silver chloride (AgCl) as the
reference electrode. The constant voltage value was set using the cell
All the experimental work were conducted twice, with the average of
potential obtained, with a scan rate of 10 mV/s. The electrodeposition
the two values calculated and reported in the results and discussion.
process was carried out for 20,000 s for each target metal sequentially,
with the working electrode replaced after each round. After the elec
trodeposition process, the working electrode was dried at 105 ◦ C over 2.2. Life cycle assessment
night and weighed. The quantity of metals recovered from the EoL solar
cell was then calculated by subtracting the final weight of the dried GaBi Professional 9.0 (Sphera Solutions GmbH) was used to conduct
working electrode with its initial weight. the life cycle assessment of the solar cell recycling process. To ensure the
Inductively coupled plasma atomic emission spectrometry (ICP-AES, accuracy of this research, a scenario was used with the experimental
PerkinElmer Optima 8000, Waltham, Massachusetts, USA) was used to study scaled up 1000 times to simulate the industrial scale, using 1000
determine and quantify the elements in the leaching solution before and waste panels, each with 400 mm ✕ 200 mm in size as the functional unit
after the electrodeposition process. The recovery efficiency of aluminum (a treatment capacity of 892.5 kg/h). The simulation was based on the
from the precipitation process was calculated using Equation (1), while GaBi database sourced from European regions, combined with results
the recovery efficiency of the electrodeposited metals was calculated acquired from this study. The system boundary used is shown in Fig. 4.
using Equation (2). The overall recovery efficiency was then calculated The end-treatments for different components of the EoL solar PV panels
via Equation (3). involved in the recycling process are listed in Table 2. Environmental
impacts were assessed in accordance with the ISO 14040 and 14044
Ci, 0 − Ci, 0
Recovery efficiency for Al, RAl (%) = × 100% (1) standards. The Centrum voor Milieukunde Leiden (CML) 2000 method
Ci, 0 was used for impact categorizations.
Fig. 4. The system boundary of the recycling process used in the life cycle assessment, with 1000 EoL monocrystalline silica solar panels of size 400 mm ✕ 200 mm
and a treatment capacity of 892.5 kg/h as the basis.
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M.S.W. Lim et al. Journal of Cleaner Production 340 (2022) 130796
Table 2 applied costs of raw materials and waste treatment, as well as the rev
The assumed end-treatments for different components of the EoL solar panels enue from the recycled products can be found in the Supplementary
involved in the recycling process. Information (Tables S15–S16), with the example calculations made
Waste components Assumed disposal method Data source available.
Steel screws Recovery and reuse GaBi 9.0 professional database
Silver Recovery and reuse 3. Results and discussion
Aluminum Recovery and reuse
Silicon wafers Recovery and reuse 3.1. Characterization of the EoL solar PV cells
Lead Recovery and reuse
Plastic Recovery and reuse
Glass Landfilling Fig. 6 illustrates the XRD diffractogram obtained for the EoL solar PV
Copper cable Recovery and reuse cell sample. As seen in the figure, peaks at 37, 44, 64 and 77◦ correspond
EVA Incineration to the crystalline peaks of monocrystalline silicon (JCPDS No. 01-089-
905), indicating and verifying that the treated sample originated from
a monocrystalline silicon solar PV panel.
In the LCA, two scenarios were evaluated, i.e. the landfilling of the
The untreated and treated EoL solar cells were examined with
EoL solar panels and the recycling of the EoL solar panels. Six impact
scanning electron microscopy, with the SEM images of the front and rear
categories were selected: global warming potential (GWP), human
side of the cells shown in Fig. 7. In Fig. 7(a), the Ag electrode can be
toxicity potential (HTP), acidification potential (AP), ozone depletion
observed on the scan of the untreated cell, represented by the white
potential (ODP), eutrophication potential (EP) and freshwater ecotox
visible strip, which contains Ag to be recovered.
icity potential (FEP). The distance of goods transportation was assumed
Fig. 7(c) shows the captured scan of the front view of the treated
to be 100 km and light duty vehicles of a Euro 5 standard with a
maximum of 1.5 t payload capacity were used in the LCA simulation.
Fig. 5. Process flow diagram for the simulated industrial-scale EoL solar PV recycling process.
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M.S.W. Lim et al. Journal of Cleaner Production 340 (2022) 130796
Fig. 7. SEM images of the (a) front side, and (b) rear side of the untreated solar cell; (c) front side, and (d) rear side of the acid-etched solar cell.
panel, with the Ag electrode strip visible, which indicates that area of electrodeposition. On the other hand, Al was recovered via precipitation
analysis taken into account by the EDX elemental analysis. and subsequent filtration of the neutralized leaching solution. Prior to
The EDX analyses of the untreated and treated EoL solar cells are electrodeposition, the cell potentials (E0) of Pb and Ag were obtained
shown in Fig. 8. From Fig. 8(a), the front end of the untreated EoL through the CV test, with the voltammetry of the leaching solution
monocrystalline silicon solar PV cell contains Pb and Ag in trace shown in Fig. 9. A bump in the figure indicates an increased cathodic
amounts, which was a result of the welding and conductor materials. On current, showing the reduction process of the particular element is
the other hand, from Fig. 8(b), it can be seen that the rear end of the taking place. Through the test, it was determined that the cell potentials
panel contains only Al from the coating material. No other metallic in for the reduction of Ag and Pb were +0.41 V and - 0.13 V respectively.
clusions were observed. The presence of oxygen was due to the exposure The equations involved for the recovery of Ag are:
of Al to the air, subsequently resulting in aluminum oxide.
Cathode : Ag+ + e− →Ag E0 = + 0.41 V (8)
After treatment, as shown in Fig. 8(c) and (d), the composition of the
elements – Pb, Ag and Al, were significantly decreased from the silicon
Anode : 2H2 O → O2 + 4H+ + 4e− (9)
wafer as they were leached out to the leaching solution.
Overall equation : 4AgNO3 + 2H2 O→4Ag + 4HNO3 + O2 (10)
3.2. Treatment of the EoL solar PV cell
While the equations involved for the recovery of Pb are:
The acid etching of Ag, Pb and Al using the leaching solution con Cathode : Pb2+ + 2e− →Pb E0 = − 0.13 V (11)
sisting of nitric acid and sulfuric acid are represented by the chemical
equations: Anode : 2H2 O → O2 + 4H+ + 4e− (12)
3H2 SO4 + 2Al → Al2 (SO4 )3 + 3H2 (4)
Overall equation : 2Pb(NO3 )2 + 2H2 O→2Pb + 4HNO3 + O2 (13)
2HNO3 + Ag → AgNO3 + NO2 + H2 O (5) Therefore, Ag was first recovered, followed by Pb. EDX analysis was
also carried out on the working electrodes before and after electrode
8HNO3 + 3Pb →3Pb(NO3 )2 + 2NO + 4H2 O (6) position to validate the recovery of the target metals, with results pre
While the subsequent neutralization of Al with NaOH represented by sented in Fig. 10. From the elemental analysis, it can be seen that the
the chemical equation: composition of Ag and Pb on the working electrodes was significantly
increased, signifying a successful recovery of Ag and Pb through elec
Al2 (SO4 )3 + 3Ca(OH)3 →2Al(OH)3 + 3CaSO4 (7) trodeposition using sequential constant voltages of +0.41 V and – 0.13
Table 3 summarizes the results of metal recovery, with the recovery V, respectively. On the other hand, Table 4 presents the quantity of the
efficiencies calculated via Equation (1) – (3) using the concentrations of metals recovered on a weight basis. The recovered Ag, Pb and Al were
the leaching solutions obtained from the ICP-AES analysis. As shown in 13.3, 6.7 and 157.6 g/kgEoL solar cell, respectively, totaling 177.7 g of
the table, the recovery efficiencies of Ag, Pb and Al were calculated to be metals recovered per kg of waste solar cell.
82%, 91% and 86% respectively, with an overall metal recovery effi In this study, the chemicals used are HNO3, H2SO4, H2O2 and NaOH,
ciency of 86%. Following acid etching, the leaching solution was further which present an advantage for industrial operations as these chemicals
treated to recover the target elements. are widely available and cost-effective. While some studies presented in
The target elements (Pb and Ag) were recovered via constant-voltage the literature utilizing solvent extraction method have higher recovery
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M.S.W. Lim et al. Journal of Cleaner Production 340 (2022) 130796
Fig. 8. EDX results of the (a) front side, and (b) rear side of the untreated solar cell; (c) front side, and (d) rear side of the acid-etched solar cell.
Table 3
Concentrations of Ag, Pb and Al in the leaching solution and their calculated recovery efficiencies.
Element, i Concentration (mg/L) Recovery efficiency (%) calculated using
Equations (1)–(3)
Leaching Neutralized leaching After electrolyzed at +0.41 V After electrolyzed at − 0.13 V
solution, Ci,0 solution, Ci,0 for Ag, Ci,V1 for Pb, Ci,V2
rates, such as those performed by Jung et al. (2016) with a Ag recovery chemicals. However, to increase the purities of the recovered metals,
rate of 90%, complex reactants such as 2-hydroxy-5-nonylacetopheno optimizing acid etching or solvent extraction method, and the sequential
neoxime (LIX 84-I) were used. Similarly, in Chen et al. (2021, 2020), electrodeposition/electrowinning, and conducting feasibility and
complex chemical agents such as Na-Cyanex 272 in kerosene and viability studies would be a promising direction (Mahmoudi et al., 2020;
2-hydroxy-5-nonylacetophenone oxime (LIX984N) were employed to Sun et al., 2015; Tao andHuang, 2018).
separate components such as Ag and Al, and to extract copper respec
tively, which add to the complexity and hence the applicability of the
3.3. Life cycle assessment (LCA)
recycling process.
In a separate study, while Chung et al. (2021) utilized an environ
The results of the LCA are shown in Figs. 11 and 12. The global
mentally friendly iodine-iodide system to extract Ag and Al, both Ag and
warming potentials (GWP) of both the recycling and landfilling pro
AI are inherently difficult to separate as both components are coexisting,
cesses of the EoL solar PV panels are shown and compared in Fig. 11, in
thus requiring special treatment for separation. Furthermore, while
which the credits observed as negative values represent the avoided
some studies present a simple process for Ag recycling, the leaching rates
impacts. The GWP is an important indicator developed to represent the
was low and the reaction time taken was rather long, i.e. 24 h (Dias
relative climate impact of different greenhouse gases or processes.
et al., 2016; Wongnaree et al., 2020). This study presents an adequate
Specifically, it is a measure of how much energy the emission of 1 tonne
leaching rate with a fast reaction time with the use of common
of a greenhouse gas will absorb over a given period of time – typically
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M.S.W. Lim et al. Journal of Cleaner Production 340 (2022) 130796
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M.S.W. Lim et al. Journal of Cleaner Production 340 (2022) 130796
Fig. 10. EDX results of the working electrode (a) before electrodeposition; (b) after electrodeposition at +0.41 V; and (c) after electrodeposition at − 0.13 V.
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M.S.W. Lim et al. Journal of Cleaner Production 340 (2022) 130796
Fig. 11. The global warming potential results of the (a) recycling process and (b) landfilling process.
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M.S.W. Lim et al. Journal of Cleaner Production 340 (2022) 130796
Fig. 12. The comparative potentials of each impact category for the recycling and landfilling method.
Table 5
Flowrate outputs for different streams on the process flow dia
gram of Fig. 5.
Component Flow rate (kg/h)
Steel 32.15
Aluminum frame 172.26
Copper 2.95
Plastic (1 and 2) 41.81
Silicon 25.20
Silver 0.41
Lead 0.21
Aluminum hydroxide 6.95
Waste solution 243.70
Table 6
Economic outputs of the simulated recycling process, at a treatment capacity of
892.5 kg/h and collection fee subsidized.
Aspect Value Unit
apply them to a life cycle assessment and compared the recycling pro
cess to a typical landfilling method to dispose waste solar panels. Among
the six impact categories studied, the global warming potential was
significantly reduced by approximately 393% when the recycling
method was applied to treat the panels. While the human toxicity po
tential is high for the recycling process due to the waste materials
emitted during the process, the impact can be mitigated by imple
Fig. 13. Breakdown of (a) revenue and (b) expenditure for the EoL solar PV
menting more efficient processing techniques to reduce and prevent the panel recycling plant.
release of toxic materials to the environment. Finally, an economic
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M.S.W. Lim et al. Journal of Cleaner Production 340 (2022) 130796
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Declaration of competing interest
%3A%2F%2Fwww.irena.org%2Fpublications%2F2021%2FMarch%2FRenewabl
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The authors declare that they have no known competing financial August 2021).
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The authors would like to thank Ministry of Science and Technology Jung, B., Park, J., Seo, D., Park, N., 2016. Sustainable system for raw-metal recovery
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(MOST), Taiwan for providing funding for this research under the grant
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110-2637-E-027 -007. acssuschemeng.6b00894.
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