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Science of the Total Environment 819 (2022) 153105

Contents lists available at ScienceDirect

Science of the Total Environment


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

Comparative life cycle assessment of LFP and NCM batteries including the
secondary use and different recycling technologies
Jiawei Quan, Siqi Zhao, Duanmei Song, Tianya Wang, Wenzhi He, Guangming Li

State Key Laboratory of Pollution Control and Resources Reuse, Shanghai Institute of Pollution Control and Ecological Security, College of Environmental Science and Engineering,
Tongji University, Mingjing Building, 1239 Siping Road, Shanghai 200092, People's Republic of China

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• A from-cradle-to-grave life cycle assess-


ment and comparison between LFP and
NCM batteries were performed.
• The resource depletion and environmen-
tal emissions of the LFP batteries were
higher.
• Environmentally, hydrometallurgy outper
formed pyrometallurgy and direct physi-
cal recycling.
• Production, first use, and secondary use
dominated the environmental impacts of
LIBs.
• Enhanced charge-discharge efficiency
helped significantly reduce environmen-
tal burdens.

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

Article history: Lithium iron phosphate (LFP) batteries and lithium nickel cobalt manganese oxide (NCM) batteries are the most
Received 1 September 2021 widely used power lithium-ion batteries (LIBs) in electric vehicles (EVs) currently. The future trend is to reuse LIBs re-
Received in revised form 9 January 2022 tired from EVs for other applications, such as energy storage systems (ESS). However, the environmental performance
Accepted 10 January 2022
of LIBs during the entire life cycle, from the cradle to the grave, has not been extensively discussed. In this study, life
Available online 15 January 2022
cycle assessment (LCA) was used to quantify and compare the environmental impacts of LFP and NCM batteries. Apart
Editor: Deyi Hou from the phases of production, the first use in EVs, and recycling, the repurposing of retired LIBs and their secondary
use in the ESS were also included in the system boundary. Also, the environmental impacts of various recycling pro-
Keywords: cesses were evaluated. The LCA results suggested that the NCM battery had better comprehensive environmental per-
Lithium-ion batteries formance than the LFP one but shorter service life over the whole life cycle. In China, the first and secondary use phases
Life cycle assessment contributed most to the environmental impacts with electricity mostly generated from fossil fuels. The LIB production
Secondary use phase was relevant to all assessed impact categories and contributed more than 50% to Abiotic Depletion Potential
Recycling (ADP elements) particularly. The environmental loads could be mitigated through the recovery of metals and other
materials. And, hydrometallurgy was recommended for recycling waste LIBs by better environmental advantages
than pyrometallurgy and direct physical recycling. Sensitivity analysis revealed that by optimizing the charge-
discharge efficiency of LIBs, particularly LFP batteries, all environmental burdens could be considerably decreased.
Therefore, improving the electrochemical performance of LIBs and increasing the use proportion of clean energy
were crucial to reduce the environmental impacts over their entire life cycle.

⁎ Corresponding author.
E-mail address: ligm@tongji.edu.cn (G. Li).

http://dx.doi.org/10.1016/j.scitotenv.2022.153105
0048-9697/© 2022 Elsevier B.V. All rights reserved.
J. Quan et al. Science of the Total Environment 819 (2022) 153105

1. Introduction industry. However, the above LCA studies did not include a complete life
cycle and could therefore not provide any information or recommendation
Global warming was intensified by the rapid development of technology regarding the environmental impact of any of the assessed battery types.
and the industrial revolution (Kamran et al., 2021). Transportation accounted Hence, studies had gradually focused on the economic and environmental
for a sizable portion of CO2 emissions (Faria et al., 2013; Sommerville et al., feasibility of repurposing and second-use of LIBs. Farian et al. (2014) dem-
2021; WRI, 2020). Therefore, electric vehicles (EVs) were being developed onstrated that the environmental implications of secondary use were highly
globally for greater environmental benefits (Crenna et al., 2021; Faria et al., reliant on the electricity mix and battery efficiency loss. Richa et al. (2017b)
2013), which was also a critical strategy for China to address global climate noted that reusing refurbished LIBs in energy storage systems (ESS) would
change and promote green development (Central People's Government of be more environmentally advantageous than manufacturing and utilizing
China, 2020). Lithium-ion batteries (LIBs) were the most frequently utilized lead-acid batteries, without specifying the type of LIBs. Ahmadi et al.
technology in EV power supply systems due to the long cycle life and high en- (Ahmadi et al., 2017; Richa et al., 2017b) discussed environmental impacts
ergy density (Alfaro-Algaba and Ramirez, 2020). In particular, lithium iron of LFP batteries throughout their entire life cycle, including manufacturing,
phosphate (LFP) batteries and lithium nickel cobalt manganese oxide EV use, remanufacturing, reuse in ESS, and recycling, while the lifetime of
(NCM) batteries were widely employed in the EVs market for their excellent the two use stages was assumed to be 18 years roughly. Yang et al. (2020)
drivability performance (Kamran et al., 2021). But LIBs were essentially evaluated the environmental feasibility of repurposing LFP batteries in
energy-intensive products leading to significant energy demand and pollution communication base stations without considering the use phase in the sys-
emissions during production and use stages. tem boundary. And Peters et al. (2017) conducted a review of LCA studies
The environmental impacts and resource demands associated with LIBs of LIBs and found that only a few publications provided original life cycle
within the life cycle were key challenges that restricted the sustainable devel- inventory data. In sum, existing researches cannot adequately capture the
opment of EVs. With the increasing amount of LIBs, the energy and resources environmental implications of China's LFP and NCM batteries across their
requirements for the production processes increased significantly (Yin et al., whole life cycle, from cradle to grave.
2016). Despite rising demand, China's lithium, nickel, and cobalt reserves This study aimed to address the gaps in environmental aspects of LIBs' en-
were comparatively small (USGS, 2020; Zhang et al., 2020). Meanwhile, tire lifecycle via innovatively proposed complete life cycle models for both
the environmental pollution associated with the battery production process LFP and NCM batteries. The battery production phase, first use (used in
couldn't be ignored (Wang et al., 2019; Wu and Kong, 2018). When the capac- EVs) phase, repurposing phase, secondary use (used in ESS) phase, and
ity decreased to 80% of the nominal capacity, the LIBs were considered to re- recycling phase were all considered in system boundaries. For the
tire from EVs for the first use phase (Fan et al., 2020). After repurposing, repurposing and recycling phases, foreground data were obtained from typi-
retired LIBs could be utilized as energy storage modules in less-demanding cal enterprises in China. As for the two use phases, the energy consumption
applications, such as peak shaving, renewable energy storage, low-speed elec- was calculated based on battery capacity decay and cycle life rather than a
tric cars, and power tools (Hua et al., 2020; Jia et al., 2018). Secondary use simple assumption of service life. Simultaneously, two different recovery pro-
was considered a cost-effective measure to delay the scrapping of LIBs, cesses were considered for LFP and NCM batteries, respectively. The objective
while also providing opportunities for energy and the environment was further to explore the environmental performance of various recycling
(Ahmadi et al., 2017; Yang et al., 2020). Therefore, the secondary use of re- technologies. Also, complete and transparent life cycle inventories were pro-
tired LIBs was viewed as a promising development trend with commercial po- vided for all lifecycle phases. The LCA results would help make judgments on
tential and environmental advantages. However, studies on environmental secondary use in the ESS. Moreover, the comparative analysis of environmen-
assessments of applications of second-life LIBs were limited to a degree. tal impacts associated with the recycling phase would aid in selecting and
The LIBs would enter the end-of-life (EoL) phase when their capacity promoting recycling technologies. Additionally, decision-making and techni-
dropped below 60% of the nominal capacity. The proper treatments of cal support were offered for related green manufacturing and full lifecycle
EoL LIBs were needed. On the one hand, EoL LIBs contained abundant management to help the power LIBs industry develop more sustainably.
metals (especially lithium, nickel, cobalt, aluminum, and copper), all of
which had a high economic value for recovery (Richa et al., 2014; 2. Data and methodology
Sommerville et al., 2021). On the other hand, metals and organics included
in EoL LIBs would trigger environmental pollution and cause pathogenic In this study, LCA was used, which has been recognized to assess prod-
risks to human health without adequate recycling (Hua et al., 2020; ucts' life-cycle environmental impacts quantitatively (Kirchain et al., 2017;
Winslow et al., 2018; Yin, 2018). Hydrometallurgy, pyrometallurgy, and di- Liang et al., 2017).
rect physical recycling were the dominating techniques of recovery (Chen LCA was carried out according to ISO 14040-2006 and ISO 14044-2006
et al., 2019). Additionally, the environmental performance of the various (ISO 14040, 2006; ISO 14044, 2006) published by the International Orga-
recycling processes remains to be analyzed. nization for Standardization (ISO). Modeling was performed by GaBi Edu-
Therefore, an assessment was required to specify the environmental im- cation, which supported several databases and was widely used for LCA
pacts of LIBs from a whole life cycle perspective. Life Cycle Assessment (Zhao et al., 2019).
(LCA) has been widely used to assess the environmental performance of
LIBs (Zhang et al., 2018) due to its ability to quantify and analyze environ- 2.1. Goal and scope definition
mental impacts along with every lifecycle phase.
It could be found that the environmental impacts of LIBs had been quan- The goals of the study were:
titatively assessed in some recent LCA studies. However, these studies (1) to establish and complete the entire life cycle inventories (LCIs) of
focused more on the battery production and first use phase in EVs LFP and NCM batteries;
(Ellingsen et al., 2014; Kim et al., 2016; Notter et al., 2010; Van den (2) to compare the environmental performance of LFP and NCM batte-
Bossche et al., 2006; Zackrisson et al., 2010). Also, the environmental per- ries from a full life cycle perspective and to confirm the environmental fea-
formance of LIBs recycling has been discussed in some studies. The study by sibility of secondary use of LIBs in ESS.
Hendrickson et al. (2015), based their dataset on the Umicore Patent No. (3) to provide comparative analyses of environmental impacts of differ-
US 7,169,206 B2 (2007), suggested that hydrometallurgy could save ent recycling technologies and to offer a reference for selecting industrial-
more energy than pyrometallurgy. Hao et al. (2017b) observed that hydro- ized recycling methods.
metallurgical recycling of NCM batteries could achieve CO2 emissions re-
duction, but the comparison of recycling technologies was not carried 2.1.1. Functional units
out. Mohr et al. (2020) quantified the potential reduction in environmental The functional unit (FU) was defined as the nominal capacity of a 1 kWh
impacts achieved by recycling according to data obtained from European battery pack. This FU had been used in related LCA studies (Matheys et al.,

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J. Quan et al. Science of the Total Environment 819 (2022) 153105

2007; Wu et al., 2021). And all collected data needed to be converted to FU (1) Battery production phase included the production and preparation of
to ensure comparable results for the environmental impacts of different bat- cathode materials as well as the mining and refining of lithium. There-
teries. It was essential for the accuracy of the calculation results. fore, the research results were more precise and accurate.
(2) The first use phase accounted for electricity losses due to the charge-
2.1.2. System boundary discharge efficiency and weight of the LIB.
The system boundary considered five main phases during the lifetime of (3) In the reuse phase, it was assumed that only the parts and components
LFP and NCM batteries (Fig. 1). There were the battery production, the first of the LIB were replaced, not the modules or cells.
use, the repurposing, the secondary use, and the recycling phase (transpor- (4) Secondary use phase: Integrating the current cascade utilization pol-
tation was not included), where: icy and relevant technology in China, this study assumed that the sec-

Fig. 1. System boundaries of (a) LFP batteries and (b) NCM batteries. Each type of LIBs had two scenarios due to two recycling technologies.

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J. Quan et al. Science of the Total Environment 819 (2022) 153105

ondary use scenario of retired LFP and NCM batteries after accurately reflect the current state of battery production in China
repurposing is the energy storage field. (Tables S4–S17).
(5) Recycling phase: EoL NCM batteries were recycled by hydrometal-
lurgy (Mathieux et al., 2017; Swain, 2017) and pyrometallurgy 2.2.2. First use phase
(Chen et al., 2019; Gaines, 2014), while EoL LFP batteries were The first use phase referred to the process that the new LIBs were used in
recycled by hydrometallurgy and direct physical recycling (Shi EVs until the capacity decreased to 80% of the initial rate capacity. The
et al., 2018a; Shi et al., 2018b). These choices were based on the tech- electricity losses in this phase included two main parts (Ellingsen et al.,
nical characteristics of batteries (Chen et al., 2019; Wang, 2018). Hy- 2017): one was caused by the battery's charge-discharge efficiency (below
drometallurgy has been widely used in the recovery of LIBs. 100%), and the mass of the battery caused the other.
However, pyrometallurgy was not used to recycle LFP batteries be-
cause of the absence of cobalt, generally (Chen et al., 2019). NCM (1) Electricity loss due to battery's charge-discharge efficiency
batteries with complex cathode materials could not yet be strictly The charge-discharge efficiency usually depended on factors such as the
sorted through direct physical recycling (Shi et al., 2018a; Shi et al., chemical composition and the operating conditions of the battery. Accord-
2018b). And, closed-loop recycling scenarios were assumed, in ing to previous studies, the charge-discharge efficiency of various LIBs
which recovered materials were considered as substitutes for the pri- ranges from 80% to 95% (Amarakoon et al., 2013; Gerssen-Gondelach
mary materials to avoid impacts from the primary production route. and Faaij, 2012; Zackrisson, 2016; Zackrisson et al., 2010). With the in-
crease of battery cycle times, the charge-discharge efficiency will gradually
decrease. Considering that two use phases of the battery were included, it
2.2. Life cycle inventory analysis
was assumed that the charge-discharge efficiency was 90% during the
first use phase. And the charge-discharge efficiency did not decrease with
The data in this paper were divided into background data and fore-
the increase of the cycle numbers to simplify the study.
ground data. The background data were primarily obtained from
The electricity losses due to charge-discharge efficiency (Ee, kWh) was
Ecoinvent, GREET, and GaBi databases. Foreground data for LIBs pro-
defined as Eq. (1):
duction, repurposing and recycling sourced from relevant research liter-
ature and the openly available environmental impact assessment
Ee ¼ F v ∙ Dv ∙ ð1 − ηk1 Þ ð1Þ
reports of typical companies in China. We reviewed and extracted de-
tailed input-output parameters to build flows and processes of produc-
where Fv indicated energy consumption limits for EVs (i.e., the amount of
tion and recycling of batteries and related materials, which followed
electricity consumed by the EV per 100 km, kWh/100 km), Dv referred to
the principles of reliability, completeness, technical representativeness,
the distance traveled in the first use phase of the EVs (km), and ηk1 was
geographic representativeness and temporal representativeness to en-
the charge-discharge efficiency of the LIB in the first use phase, which
sure data quality (Salemdeeb et al., 2021; Weidema et al., 2013). The
took the value of 90%.
detailed foreground data would be disclosed in Section 2.2.1,
Section 2.2.3, and Section 2.2.5. (2) The electricity losses needed to carry the battery
It was assumed that the complete lifecycle phases occurred in China, Another part of the electricity losses in the first use phase was the driv-
and the average power mix in China was used (the relevant electricity ing energy consumption due to the battery mass. And the electricity losses
data referred to GaBi education China's power mix in 2016). In Sections needed to carry the battery (Em, kWh) could be defined as in Eq. (2).
2.2.1–2.2.5, the authors compiled and constructed detailed LCIs for LFP
and NCM batteries. Em ¼ k ∙ F v ∙ Dv ∙ ðm=M Þ ð2Þ

2.2.1. Battery production phase where: k denoted the powertrain apportionment factor, which indicated the
The bill of materials (BoMs) for LFP and NCM batteries was sourced ratio of the vehicle's energy consumption related to the car weight
from Dai et al., which was based on Argonne's Battery Performance and (Zackrisson et al., 2010); m was the mass of the LIB (kg), and M was the
Cost (BatPac) model (Dai et al., 2018). A total mass of 203.1 kg has been se- mass of the EV (kg).
lected for the LFP batteries and 164.99 kg for the NCM batteries. Both LIBs In this analysis, the value of k was taken as 0.49 by combining the re-
had a nominal capacity of 23.5 kWh. The BoMs for the studied LFP and sults of Kim et al. (2015) in conventional vehicles and the revised value
NCM pack were shown in Table S1. And the detailed information on the en- in EVs by Yin (2018). The value of Fv was related to the mass of the EV
ergy and water consumption of LIBs manufacturing processes was obtained and the LIB. Consequently, the Fv was assumed to be 13.1 kWh/100 km
from a published study conducted by Dai et al. (2017). The data of the study (Table S18). Also, Dv was assumed to be 200,000 km based on previous re-
were collected from one leading Chinese LIB manufacturer. search (Helmers et al., 2020; Zackrisson et al., 2010). Substituting the
The battery production process included three main parts: electrode above parameters into Eqs. (1) and (2), Ee, Em and the total electricity losses
preparation, cell production, and battery assembly. Apart from the differ- in the first use phase were calculated, as shown in Table S19. The various
ences in electrode materials, the core processes of the LFP and NCM batte- parameters related to the LFP and NCM battery systems and the equipped
ries production process were primarily the same. EVs were shown in Tables S20–S21. The LCI data for the first use phase
The battery pack assembly process didn't involve energy-intensive pro- were shown in Tables S22–S23.
cesses like cooling or drying (Dai et al., 2017). Therefore, it was assumed
that the energy consumption for battery pack assembly was negligible com- 2.2.3. Repurposing phase
pared with that for cell production. In summary, the energy consumption Repurposing was an unavoidable process for retired LIBs before second-
for LFP and NCM battery manufacturing was estimated to be 170 MJ/ ary use (Ardente et al., 2018). Typically, retired LIBs at this phase under-
kWh battery produced, of which 30 MJ was electrical energy and the re- went disassembly, inspection and assembly, cleaning, spot welding, laser
maining 140 MJ was heat, assumed for natural gas. In addition, the water welding, and assembly (Wang, 2018). However, disassembly to the module
consumption for LIBs production was 8.6 gal/kWh battery produced. Simi- or cell level depended on specific application requirements. The data of LFP
larly, the water consumption of the battery pack assembly process was neg- batteries' repurposing process (Table S24) was obtained from the project
ligible (Dai et al., 2017; Ellingsen et al., 2014). with an annual output of 120,000 sets of energy storage batteries, located
Therefore, the energy and material consumption for the production in Hebei province, China (Hebei Kui Xing New Energy Technology Co.,
phase of LIBs were presented in Tables S2–S3. Meanwhile, data on cathode 2020). The products of the project would be supplied to China Tower Cor-
active materials and precursors were primarily derived from environmental poration Limited, the world's largest telecommunications tower infrastruc-
impact assessment reports of typical Chinese facilities in order to more ture service provider, for Echelon use and power backup. And the LIBs

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J. Quan et al. Science of the Total Environment 819 (2022) 153105

dismantling and cascade utilization project in Zhuhai city provided the data purification solution. For simplicity, this paper converted the solution to
for the NCM battery repurposing phases (Zhuhai Zhongli New Energy lithium chloride solids according to the concentration. The specific inven-
Technology Co., 2019). The remanufacturing system was built in 2019 tory data was shown in Table S26.
with an annual capacity of 20,000 tons of repurposed batteries (Table S25).
b) Direct physical recycling
2.2.4. Secondary use phase Direct physical recycling was another technology for LIBs recovery.
After repurposing, the retired LIB could be reused as an energy storage Wang (2018) provided the essential foreground data obtained from a repre-
battery in the ESS of communication base stations. That was the secondary sentative company of physical recycling in Beijing. Spent LFP batteries
use phase. were automatically and finely disassembled after being discharged. Theo-
In the secondary use phase, the LIB capacity would continue to decay as retically, the cathode and anode materials, hardware, aluminum, copper,
the battery ages, and the corresponding energy efficiency would also con- electrolyte, and waste separator could be recovered, respectively. Then
tinue to decay (Ahmadi et al., 2014). However, the decay of energy effi- the cathode and anode materials would be used in the production and
ciency increased the study's complexity and was not accounted for in this manufacturing of batteries after being repaired. The specific inventory
study to simplify the calculations. Although the performance of the data was shown in Table S27.
repurposed LIBs had not been widely studied (Tao et al., 2017), previous re- (2) Recycling process and inventory of EoL NCM batteries
search had shown that the capacity loss of LIBs was dependent on the num-
ber of cycles (Arora et al., 1998). Therefore, the semi-empirical model a) Hydrometallurgy
proposed by Han et al. (2014) was used here to estimate the capacity loss The hydrometallurgy of waste NCM batteries mainly included pretreat-
of LIBs. The model was convenient for calculating the electricity loss of ment, leaching, precipitation, and sintering. Finally, NCM ternary cathode
the LIB because LIBs did not have to be tested in advance. The LIB capacity materials were obtained, as well as aluminum, copper, steel, and other
loss of each cycle (ξ) was defined in Eq. (3): metals. Aluminum was recovered at a relatively high rate in this technique.
Due to the fact that the aluminum foil was separated from the battery active
ξ ¼ A ∙ exp−ðEa =RtÞ ∙ nz ð3Þ
material following pyrolysis. The LCIs of hydrometallurgy were obtained
from a published research conducted by Xie et al. (2015), as shown in
where A was a constant, Ea denoted the activation energy (J·mol−1), R rep-
Table S28. The data of the study were collected from a leading battery
resented the gas constant (J·mol−1·K−1), t referred to the thermodynamic
recycling enterprise, owned by the world's top three LIB suppliers, in
temperature, n was the cycle life (not counted if it cannot undergo a com-
Foshan city, Guangdong province.
plete charging and discharging process), and z represented the power-law
factor. b) Pyrometallurgy
For the LFP battery, the parameters of the LIB model proposed by Han The waste NCM battery was crushed initially and then smelted, blown,
et al. (2014) were used: the values of A, Ea/Rt, z and t were set to 0.1825, ground, floated, cast anode, electrolytic refining, dissolution, precipitation,
1324.65, 0.5878, and 298.15 K (25 °C), respectively. and sintering. The final products were NCM ternary cathode materials. This
For the NCM battery, the parameters of the LIB model proposed by Li process consumed a lot of energy.
et al. (2016) were used: simplified A ∙ exp−(Ea/Rt) to the constant B and The inventory data of pyrometallurgy of EoL NCM batteries were based
took the values of B and z as 0.00362 and 0.588, respectively. on the study of Xie et al. (2015), as shown in Table S29.
In the secondary use phase, only electricity losses owing to the internal Waste BMS, steel scrap, aluminum scrap, copper scrap, plastic scrap,
efficiency of the battery and transmission efficiency were included (Richa graphite scrap, etc., generated in the recycling process were further regen-
et al., 2017b). According to Yang et al. (2020) and Richa et al. (2017b), erated. The obtained recycled materials would be used in the battery pro-
the electricity losses (Eloss, kWh) in the secondary use phase of LIBs were es- duction phase. The detailed regeneration process and inventory data were
timated from the start of use in the ESS (n = 1) to the EoL (n = lc), which listed in Tables S30–S33. Other solid wastes were treated by incineration
were defined as in Eq. (4): and landfill in accordance with general municipal waste, and the specific
process referred to GaBi's database.
X
lc
Eloss ¼ E ∙ ð1 − ξÞ ∙ DoD ∙ ð1 −ηT ∙ ηk2 Þ=ðηT ∙ ηk2 Þ ð4Þ
n¼1 2.3. Life cycle impact assessment

where E represented initial capacity of the secondary use phase of LIBs The whole lifetime of LIBs was modeled and calculated by GaBi Educa-
(kWh), DoD was the depth of discharge, ηT indicated the transmission effi- tion. And the environmental impact assessment was performed by CML
ciency, and ηk2 was the charge-discharge efficiency. 2001, which included characterization, normalization, and weighting.
Combining with the actual level of China's power grid (Yin, 2018) and CML2001 was a problem-oriented method that could reflect the direct
the existing relevant research assumptions (Ahmadi et al., 2017), this impact of the life cycle on the environment (Fernandez-Marchante et al.,
paper set the DoD, ηT, and ηk2 as 80%, 90% and 85%, respectively. 2020). It quantifies the results into multiple impact categories at the mid-
According to a related study (Yang, 2019), this paper assumed that LIBs point level. This method was also widely used in LCAs about LIBs (Choma
entered the end of secondary use life and were recycled when their capacity and Ugaya, 2017; Marques et al., 2019).
dropped to 60% of their nominal capacity. In order to avoid problem shifting, multiple impact categories were
covered. Seven environmental impact indicators were taken in this paper,
2.2.5. Recycling phase which were: Abiotic Depletion (ADP elements), Abiotic Depletion (ADP
(1) Recycling process and inventory of EoL LFP batteries fossil), Global Warming Potential (GWP), Acidification Potential (AP),
Eutrophication Potential (EP), Ozone Layer Depletion Potential (ODP),
a) Hydrometallurgy and Photochemistry Ozone Creation Potential (POCP). The impact of
Foreground data for the hydrometallurgical recovery were collected every substance emitted into the environment hereby could be attributed
from a waste LIBs recycling project with the LFP recycling capacity of to one out of the above-mentioned seven impact categories, which have
10 kt/year in Anhui province (Anhui Daoming Energy Technology Co., been internationally agreed upon (Müller et al., 2014).
2020). The completely discharged EoL LFP batteries were dismantled, The results were then compared with previous studies and sensitivity
crushed, and sieved to obtain LFP powder. After that, the powder was analyses were performed to test the reliability and robustness of our results.
acid leached, iron removal, transformation de-hybridization, and hydro- Based on a review of the studies, results focused on GWP were compared, as
chloric acid distillation recovery, etc., to get the lithium chloride it is the only fully reported impact category. Moreover, the comparison of

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J. Quan et al. Science of the Total Environment 819 (2022) 153105

GWP was based only on the production phase, since this was generally the repurposing phase, secondary use phase (used in ESS),
phase more precisely assessed. Because LCA results in production were less recycling phase (pyrometallurgy).
affected by changes in assumptions (Cusenza et al., 2019).

And in the following, positive values represented the environmental


2.4. Sensitivity analysis
burden due to energy and resource consumption, and pollutant emissions,
while negative values indicated the environmental benefit due to the recov-
The sensitivity analysis was introduced to quantify the fluctuations in
ered materials.
LCA results caused by changes of some parameters (Gu et al., 2019).
And the following four parameters were considered, which were:
3.1.1. Abiotic resource depletion impacts
(1) Energy consumption in the battery production phase (Ep); (1) Abiotic Depletion (ADP elements)
(2) Charge-discharge efficiency in the first use phase (ηk1); As shown in Fig. 2a, the battery production phase was the primary con-
(3) Energy consumption limits for the first use phase (Fv); tributor to ADP elements (ADPe). And the contribution of the NCM battery
(4) Charge-discharge efficiency in secondary use phase (ηK2). was slightly lower than that of the LFP battery. Due to the lower energy den-
For all the selected parameters, simulations are conducted in 10% in- sity of the LFP battery, it required more LFP cathode material and various
creasing and 10% decreasing of the value in base case for comprehensive metals for the same functional unit conditions (Yu et al., 2018). For LFP bat-
analysis. teries, either hydrometallurgy or direct physical recycling could offset a cer-
The above four sensitivity factors were all related to the energy con- tain amount of ADPe. However, for NCM batteries, only hydrometallurgy
sumption of the whole lifetime of LIBs. These parameters were also of cur- provided considerable mineral resource benefits, whereas pyrometallurgy
rent concern in batteries' production and use phases. provided negligible environmental benefits. Because the steel, copper,
Studies had shown that the environmental impact of the battery produc- and aluminum in NCM batteries were not well recycled by the pyrometal-
tion phase was strongly related to energy consumption. The charge- lurgy. And a quantity of lithium carbonate was consumed to regenerate
discharge efficiency of a battery was closely associated with its internal the cathode material.
performance and determined the energy loss in the process of use. There- (2) Abiotic Depletion (ADP fossil)
fore, changes in battery charge-discharge efficiency might significantly
influence the impact indicators, which could not be ignored when assessing Fig. 2b showed that the ADP fossil (ADPf) of LIBs was mainly concen-
the environmental impact (Peters et al., 2017). The energy consumption trated in the battery production, first use, and secondary use phases. The
limit was related to the design of the EV, like curb weight. The energy con- battery production phase consumed a great deal of energy such as coal,
sumption limit also affected the electricity consumption of the LIBs during oil, and electricity to manufacture metals like steel, aluminum, lithium,
the first use phase. and cobalt. And the first and secondary use phases mainly consumed elec-
tricity. China was still dominated by coal power, which accounted for
65% of the electric power structure in 2016 (China Energy Portal, 2016).
3. Results and discussions
Hence the two use phases were the primary contributors to ADPf. And
the ADPf of the secondary use phase was obviously higher than that in
3.1. Characterization results of environmental impact indicators
the first use phase, especially for the LFP batteries. Because in the sec-
ondary use phase, the LIB would charge and discharge repeatedly until
Depending on the types of battery and recycling process, four scenarios
the remaining capacity decays to 60% of the nominal capacity
were included, as follows:
(Ioakimidis et al., 2019). Therefore, it had experienced more charge
Scenario 1: LFP battery production phase, first use phase (used in EV), and discharge cycle numbers than the first use phase. Moreover, the ex-
repurposing phase, secondary use phase (used in ESS), cellent capacity retention performance of the LFP battery allowed it to
recycling phase (hydrometallurgy). be cycled 3275 times in the secondary use phase, which was about 2.4
Scenario 2: LFP battery production phase, first use phase (used in EV), times that of the NCM battery. For all scenarios, the environmental ben-
repurposing phase, secondary use phase (used in ESS), efits associated with materials recovered through battery recycling pro-
recycling phase (direct physical recycling). cesses exceed the associated environmental burdens linked to the
Scenario 3: NCM battery production phase, first use phase (used in EV), recycling process in ADPf. And the environmental benefit of hydromet-
repurposing phase, secondary use phase (used in ESS), allurgy was significantly higher than that of direct physical recycling
recycling phase (hydrometallurgy). and pyrometallurgy. In general, compared with NCM batteries, LFP bat-
Scenario 4: NCM battery production phase, first use phase (used in EV), teries generated the severer burden of ADPf.

Fig. 2. Comparisons of resource depletion potential of per kWh LFP and NCM battery pack: (a) Abiotic Depletion (ADP elements), and (b) Abiotic Depletion (ADP fossil).

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This study-NCM batteries production practices. Besides, diversity in data collection channels
This study-LFP and background datasets during the battery production phase might also
Sun et al., 2020-NCM lead to differences in results, which was worth exploring in the future.
Dai et al., 2019-NCM
Hao et al., 2017-NCM
(2) Acidification Potential (AP)
Hao et al., 2017-LFP As shown in Fig. 4b, the positive values of AP were mainly concentrated
Kim et al., 2016-LMO+NCM in the battery production and two use phases, and the contribution of the
McManus, 2012-LFP repurposing phase was minimal. The AP of the LFP battery in the secondary
Majeau-Bettez et al., 2011-LFP use phase was still the highest, which was related to the electricity consump-
Majeau-Bettez et al., 2011-NCM tion in this phase. The coal-fired power generation was the main body of
Zackrisson et al., 2010-LFP
China's electricity structure, leading to the emission of numerous acidifying
gases like SO2 and NOX (Yu et al., 2018). Nonetheless, the AP of the NCM bat-
0 50 100 150 200 250 300
tery in the production phase was greater than that of the LFP battery (Majeau-
kg CO2 eq./kWh battery production Bettez et al., 2011) because of the higher nickel and cobalt content rates. The
smelting process of these metals generated high levels of sulfur oxides, which
Fig. 3. Comparison of per kWh LIB production among research findings. would lead to the formation of acidification. Therefore, recycling the ternary
cathode material from EoL LIBs could avoid the environmental impacts in the
3.1.2. Environmental emissions impacts upstream acquisition phase of primary nickel and cobalt resources. Thus, the
(1) Global Warming Potential (GWP) negative value of AP in the recycling phase indicated that, the recycling pro-
cess has some environmental benefits. For LFP batteries, the environmental
As shown in Fig. 4a, the GWP of LIBs had a high correlation with the dis- benefits of hydrometallurgy mainly came from the secondary lithium chlo-
tribution of the abiotic depletion (fossil). Owing to the large amounts of ride generated in the recycling phase. As for NCM batteries, the hydrometal-
CO2 emitted by coal-fired power generation, the contribution to GWP of lurgical and pyrometallurgical recycling had obvious environmental benefits
two use phases exceeded 60%. The secondary use phase of LFP batteries due to the regeneration of cathode materials. Overall, the AP of LFP batteries
with the highest GWP was 441 kg CO2 eq., accounting for approximately is higher than that of NCM batteries.
41% of the whole life cycle. The GWP of the NCM battery during the sec- (3) Eutrophication Potential (EP)
ondary use phase was much smaller, only 181 kg CO2 eq. And the GWP As shown in Fig. 4c, the EP of all life cycle phases was positive except for
of the repurposing phase was very inconspicuous. the hydrometallurgical recycling process of the LFP battery. The environ-
The GWP of LFP and NCM batteries production phase in our findings was mental benefit (about EP) was obtained due to the generation of lithium
compared with existing studies in Fig. 3 (Dai et al., 2019; Hao et al., 2017a; chloride from the hydrometallurgy of LFP batteries. In contrast, the envi-
Kim et al., 2016; Majeau-Bettez et al., 2011; McManus, 2012; Sun et al., ronmental burden (about EP) for the hydrometallurgical recycling process
2020; Zackrisson et al., 2010). Our results of GWP for LFP and NCM batteries of NCM batteries was created. Given the fact that the hydrometallurgy of
production phase (76.7 kg CO2 eq. and 87.1 kg CO2 eq.) were in the midrange NCM batteries involved a significant amount of ammonia which triggered
of literature estimates (61–266 CO2 eq. and 72.9–140 kg CO2 eq.). Distinc- large impact in EP. And the contribution to the EP of the repurposing
tions from existing results could be attributed to the differences in battery de- phase in all scenarios was almost zero.
sign and energy consumption. The GWP in the LFP battery production phase
determined by Zackrisson et al. (2010) and Majeau-Bettez et al. (2011) were (4) Ozone Layer Depletion Potential (ODP)
over three times higher than this study. Their data based on laboratory trials As shown in Fig. 4d, the positive ODP values were mainly concentrated
or industry reports published over 10 years might not reflect current LFP in the battery production and two use phases. The ODP of the battery

Fig. 4. Comparison of the environmental emissions of per kWh LFP and NCM battery packs: (a) Global Warming Potential, (b) Acidification Potential, (c) Eutrophication
potential, (d) Ozone Layer Depletion Potential, and (e) Photochemistry. Ozone Creation Potential.

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J. Quan et al. Science of the Total Environment 819 (2022) 153105

production phase was primarily due to the copper produced by electrolytic. 2019). GWP was the dominant environmental impact indicator because
And the ODP of the two use phases was still caused by electricity generated of the massive CO2 emissions from electricity generation by coal combus-
by coal combustion. For LIBs recycling, there was some environmental ben- tion (Chen, 2016). It contributed 37.14%, 38.31%, 31.05%, and 35.94%
efit (about ODP) obtained due to the mental (copper) recovery and NCM to the total environmental impacts of Scenario 1, Scenario 2, Scenario 3,
cathode material regenerated. For the same functional unit, the environ- and Scenario 4, respectively. Overall, the LFP battery featured the highest
mental benefit of ODP generated by the hydrometallurgy of LFP batteries environmental load during the entire life cycle.
was almost double that of NCM batteries. However, the repurposing
phase contributes very minimally to the ODP. But overall, the whole life- 3.2.2. Contributions of life cycle phases
time ODP of LFP batteries was higher than that of NCM batteries. In summary, the hydrometallurgy of LIBs was more environmentally
friendly. Therefore, based on the characterization results, the entire life
(5) Photochemistry. Ozone Creation Potential (POCP)
cycle phases and various categories of environmental impacts of the LIBs
As shown in Fig. 4e, the positive values of POCP were also mainly dis- recycled by the hydrometallurgy were further analyzed, as shown in Fig. 6.
tributed in the battery production and two use phases, and the negative The LFP and NCM battery production phase was the primary contribu-
values appear only in the recycling phase, with little contribution from tor to ADPe, accounting for 51% and 58% of the total value, respectively.
the repurposing phase. The POCP of NCM battery production was a little For NCM batteries, the battery production phase contributed 18%–32% to
higher than that of LFP batteries, while the POCP of LFP batteries secondary such categories as POCP, GWP, AP, ADPf, and ODP, while 9% to EP. As
use phase was roughly two twice that of NCM batteries. The highest POCP for LFP batteries, the battery production phase accounted for 9%–21% of
value was found in the secondary use phase of LFP batteries. Since that, the the total POCP, EP, GWP, AP, ADPf, and ODP.
environmental impact substances of POCP were mainly HC, NMVOC, and The LFP battery two use phases contributed 63%–84% to such catego-
CO, which were the primary air pollutants emitted during coal mining ries as ODP, ADPf, AP, EP, GWP, and POCP, while 1% to ADPe. And the
and coal-fired power generation (Wu, 2011). As for the recycling phase of NCM battery two use phases were also the major contributors to ODP,
LIBs, the environmental benefit (about POCP) was obtained due to the lith- ADPf, AP, POCP, and GWP, sharing 54%–76% of their life cycle impacts.
ium chloride and ternary cathode materials recovery. Overall, the POCP of Since electricity use was the only considered impact source during the
LFP batteries was higher than that of NCM batteries. LIBs' first and secondary use phases, the environmental burdens from
LIBs' two use phases were mainly associated with the China grid power gen-
3.2. Comparative and contribution analysis of environmental impacts eration. Thus, to reduce the environmental impacts of LIBs, the power gen-
eration and proportion of clean energy should be increased immediately.
3.2.1. The comprehensive value of different environmental impacts indicators Repurposing phases of both types of LIBs caused the least environmen-
Further normalizing and quantifying the characterization results tal impact. It indicated that repurposed retired LIBs were more environmen-
(Section 3.1), the comprehensive environmental impacts of LIBs in different tally friendly compared with producing new LIBs. The LCA results
scenarios could be obtained. As shown in Fig. 5, the comprehensive envi- suggested that the reuse of spent LIBs in ESS can provide environmental
ronmental impact value of the entire life cycle indicated that Scenario 2, benefits by avoiding the burden of manufacturing new LIBs (Richa et al.,
Scenario 1, Scenario 4, and Scenario 3 were arranged in descending 2017a).
order. The main reason was that hydrometallurgy had more significant en- In the recycling phase, the hydrometallurgy of waste LIBs had obvious
vironmental benefits than either pyrometallurgy or direct physical environmental benefits to almost each environmental impact type. Signifi-
recycling. The comprehensive environmental load of Scenario 2 was 1.6 cantly, LIBs hydrometallurgical recycling process can reduce more than
times that of Scenario 3. And the comprehensive environmental load of Sce- 40% of the life cycle ADPe. The only exception was the EP impact, where
nario 1 was 43.51% higher than that of Scenario 3. These indicated that the a considerable 45% impact share was observed. Because the NCM battery
comprehensive environmental performance of NCM batteries was better was treated by hydrometallurgy, which involved a large amount of ammo-
than that of LFP batteries. For Scenarios 1, 2, and 3, the environmental im- nia, it triggered a significant impact in EP. Overall, the entire life cycle en-
pact indicators presented in descending order were GWP, ADPf, AP, POCP, vironmental burden of LIBs was higher than the environmental benefit.
ADPe, EP, and ODP. However, for Scenario 4, ADPe was followed by GWP We compared the cradle-to-grave environmental impacts of LFP batte-
and ADPf. Because compared with hydrometallurgy, the pyrometallurgy of ries and NCM batteries with different recycling technologies. Except for
NCM batteries was ineffective in recovering various metals (Chen et al., the EP and ADPe, all other impact categories for the whole life cycle of
LFP batteries were larger than that of NCM batteries. Simislarly, the first
and secondary use phases had the most important contributions to environ-
mental impact categories other than EP and ADPe. And the contribution of
LFP batteries was always higher than that of NCM batteries. Therefore,
from the environmental point of view, extending the service life of LIBs
did not necessarily have better environmental advantages unless the elec-
tricity consumed during the two use phases came from clean energy
(Ahmadi et al., 2017). The environmental benefits of recycling were signif-
icant. For LFP batteries, the hydrometallurgical recycling process helps re-
duce all mentioned environmental burdens. It was more environmentally
friendly than direct physical recycling. The benefits of hydrometallurgical
recycling of NCM batteries were always higher than those of pyrometal-
lurgy for all impact categories, except EP.

3.3. The results of sensitivity analysis

The results of sensitivity analysis were given in Tables S34–S35, and the
±10% variation in four parameters of Scenarios 1 and 3 were carried out.
It was found that the battery production energy consumption was not
sensitive to the environmental impact results, particularly for ADPe. Com-
Fig. 5. Comparison of the comprehensive value of different environmental impact pared to other studies (Ellingsen et al., 2014; Kim et al., 2016), this paper
indicators of the entire life cycle for four LIBs scenarios. assumed a lower energy consumption of 170 MJ/kWh battery produced

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J. Quan et al. Science of the Total Environment 819 (2022) 153105

Fig. 6. Contribution of life cycle phases to environmental impacts. The recycling process was hydrometallurgy.

(Dai et al., 2019). Under current conditions, a ±10% change in battery pro- The LCA results indicated that for both types of LIBs, battery produc-
duction energy consumption cannot considerably alter battery production tion, first use, and secondary use phases posed the greatest environmental
energy intensity. As a result, it will have little effect on ADPe. Compara- loads, which could be mitigated through recycling. However, recycling by
tively, changing the energy consumption limit had a more significant effect hydrometallurgy could mitigate more environmental impacts compared
in all the environmental impact categories except ADPe. ADPf, AP, GWP, to pyrometallurgy and direct physical recycling. The environmental bur-
ODP, and POCP were more affected by changes in the energy consumption dens of the repurposing phase were much smaller than those of the battery
limit for NCM batteries than for LFP batteries. However, the sensitivity of production phase. It suggested that the reuse of retired LIBs could provide
the energy consumption limit to ADPe was not noticeable. Because chang- environmental benefits by avoiding the burdens of manufacturing new
ing the energy consumption limit by ±10% had no major impact on the LIBs.
electricity consumption during the first use phase. And the coal-fired Moreover, the comprehensive environmental impacts of LFP batteries
power generation process contributed little to the depletion of metal re- were more significant than those of NCM batteries. In particular, the elec-
sources. By reducing the weight of EVs and LIBs to decrease energy con- tricity structure in China was dominated by coal-fired power. Because the
sumption while driving, the environmental burden of LIBs might be total power consumption of the LFP battery in the two use phases far ex-
successfully mitigated. The parameters that caused the largest variation of ceeds that of the NCM battery. And LFP batteries had approximately 1.8
results were the charge-discharge efficiency in the first and secondary use times the environmental impact of NCM batteries during the two use
phases, affecting the LIBs' performance in all impact categories. Assuming phases. However, it must be noted that the long secondary service life of
that the −10% variation of charge-discharge efficiency in the secondary LFP batteries was the advantage for reuse. Therefore, it was critical to im-
use phase, the impacts would increase by 2%–32% for LFP batteries and prove the electrochemical performance of LIBs and increase the usage of re-
1%–21% for NCM batteries depending on impact categories. And the im- newable energy sources (such as hydropower and wind power). In other
pacts could be decreased by 2%–27% for LFP batteries and 0.6%–17% for phases, the environmental impacts of LFP batteries and NCM batteries
NCM batteries when the charge-discharge efficiency in the secondary use were not much different.
phase increased by 10% theoretically. For ADPf, AP, GWP, ODP, and The sensitivity analysis results showed that the charge-discharge effi-
POCP, a 10% variation of charge-discharge efficiency in the first use ciency of the battery's first and secondary use phases had a more significant
phase could reduce the impacts by 9%–20% depending on LIBs types. In effect on the LCA results.
conclusion, there was a need to enhance the research on the internal To reduce the environmental impacts of LIBs and to promote the
charge/discharge mechanism of power LIBs. The lifecycle impacts could secondary use of LIBs, suggestions were made in four aspects. Firstly, the
be significantly reduced by improving the battery technology to increase proportion of renewable energy generation in China could increase. Sec-
the charge-discharge efficiency in the two use phases. ondly, the charge-discharge efficiency and energy density of power LIBs
need to be further improved. In addition, the design of power LIBs should
4. Conclusion and suggestion be adjusted and standardized according to meet repurposing and secondary
use requirements. Finally, NCM batteries could be promoted to the market,
In this study, a detailed LCA was conducted to quantitatively analyze and hydrometallurgy was recommended for recycling.
the environmental impacts of LFP and NCM batteries throughout their en-
tire life cycle. And the battery production phase, first use (for EV) phase, CRediT authorship contribution statement
repurposing phase, secondary use (for ESS) phase, and recycling phase
were all included in the system boundary. The sensitivity analysis of energy Jiawei Quan: Conceptualization, Methodology, Data curation, Writing –
consumption in the battery production phase, energy consumption limits original draft, Visualization. Siqi Zhao: Investigation, Writing – review &
for the first use phase, and charge-discharge efficiency in the first and sec- editing. Duanmei Song: Validation, Data curation. Tianya Wang:
ondary use phases was also presented. Investigation, Writing – review & editing. Wenzhi He: Supervision,

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J. Quan et al. Science of the Total Environment 819 (2022) 153105

Conceptualization, Writing – review & editing. Guangming Li: Supervi- Fan, Z., Qiao, D., Cui, H., 2020. Influence of charge and discharge rate on capacity fade of lith-
ium ion battery. Chin.J.Power Sources 44, 325–329. https://doi.org/10.3969/j.issn.
sion, Project administration. 1002-087X.2020.03.006.
Faria, R., Marques, P., Garcia, R., Moura, P., Freire, F., Delgado, J., et al., 2014. Primary and
secondary use of electric mobility batteries from a life cycle perspective. J. Power Sources
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Faria, R., Marques, P., Moura, P., Freire, F., Delgado, J., de Almeida, A.T., 2013. Impact of the
electricity mix and use profile in the life-cycle assessment of electric vehicles. Renew. Sus-
The authors declare that they have no known competing financial inter-
tain. Energy Rev. 24, 271–287. https://doi.org/10.1016/j.rser.2013.03.063.
ests or personal relationships that could have appeared to influence the Fernandez-Marchante, C.M., Millán, M., Medina-Santos, J.I., Lobato, J., 2020. Environmental
work reported in this paper. and preliminary cost assessments of redox flow batteries for renewable energy storage.
Energy Technol. 8, 1900914. https://doi.org/10.1002/ente.201900914.
Gaines, L., 2014. The future of automotive lithium-ion battery recycling: charting a sustainable
Acknowledgment course. Sustain.Mater. Technol. 1, 2–7. https://doi.org/10.1016/j.susmat.2014.10.001.
Gerssen-Gondelach, S.J., Faaij, A.P.C., 2012. Performance of batteries for electric vehicles on
This study was financially supported by the Funding of Shanghai Insti- short and longer term. J. Power Sources 212, 111–129. https://doi.org/10.1016/j.
jpowsour.2012.03.085.
tute of Pollution Control and Ecological Security (HJGFXK-2017-002). Gu, F., Zhang, W., Guo, J., Hall, P., 2019. Exploring “Internet+Recycling”: mass balance and
The authors would like to thank the editor and anonymous reviewers for life cycle assessment of a waste management system associated with a mobile application.
supplying their valuable comments. Sci. Total Environ. 649, 172–185. https://doi.org/10.1016/j.scitotenv.2018.08.298.
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Hao, H., Mu, Z., Jiang, S., Liu, Z., Zhao, F., 2017a. GHG emissions from the production of
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