Research Article

Cite This: ACS Sustainable Chem. Eng. 2019, 7, 5082−5094 pubs.acs.org/journal/ascecg

Comparative Life-Cycle Assessment of Li-Ion Batteries through

Process-Based and Integrated Hybrid Approaches
Shipu Zhao and Fengqi You*
Systems Engineering, College of Engineering, Cornell University, Ithaca, New York 14853, United States
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ABSTRACT: This paper analyzes and compares the life cycle environmental impacts of two major types of Li-ion batteries
using process-based and integrated hybrid life-cycle assessment (LCA) approaches. The life cycle inventories (LCIs) of Li-ion
battery contain component production, battery assembly, use phase, disposal and recycling and other related background
processes. For process-based LCA, 17 ReCiPe midpoint environmental impact indicators and three end point environmental
impact indicators are considered. As for the integrated hybrid LCA study, life cycle greenhouse gas (GHG) emissions and
energy consumption are emphasized. Furthermore, we perform sensitivity analysis of life cycle GHG emissions with respect to
the uncertainties in product prices, mass of BMS and cooling system, and production efficiency. The integrated hybrid LCA
results show that battery cell production is the most significant contributor to the life cycle GHG emissions and the economic
input-output (EIO) systems contribute the largest part in life cycle energy consumption for both types of Li-ion batteries. The
most significant difference between two Li-ion batteries lies in the disposal and recycling stage. For LiMn2O4 (LMO) battery,
the disposal and recycling stage only makes up a small portion of less than 10% for life cycle GHG emissions and energy
consumption. However, for Li(NixCoyMnz)O2 (NCM) battery, it contributes a significant part at more than 20%.
KEYWORDS: Li-ion battery, Integrated hybrid life cycle assessment, Environmental impacts

■ INTRODUCTION
Along with the rapid development of battery-powered electric
vehicle industry, electrochemical energy storage has gained
increasing attentions. 1,2 Li-ion battery is an attractive
technology for electrochemical energy storage due to its
features of high energy density, enhanced rate capabilities and
long service life.3 It has been a very active area of research to
develop novel and advanced rechargeable Li-ion batteries.
However, the production, use and disposal of Li-ion batteries
may lead to environmental burdens, and there are very few
studies about the corresponding environmental impacts.
Currently, most LCA studies about battery technologies are
conducted on traction batteries as part of electric vehicles.4−6
Batteries used for hybrid electric vehicles, and plug in hybrids
have been studied to the largest extent in recent years.6
Therefore, it is important to quantitatively investigate the
environmental impacts of Li-ion batteries from a life cycle
perspective.
Commercial Li-ion batteries use various types of cathode
materials, including LiMn2O4 (LMO), LiFePO4 (LFP),
Li(NiCoAl)O2, and Li(NixCoyMnz)O2 (NCM), where x, y,
and z denote different possible ratios.7,8 As for anode material,
graphite is commonly adopted regardless of different cathode
materials.9−11 Different combinations of cathode and anode
materials have different properties and may result in different
performances, such as energy density and lifetime. The
comparison of life cycle environmental impacts between
different types of Li-ion batteries could help to identify the
environmental “hotspot” and provide recommendations to
future development of Li-ion battery technologies. Existing
LCA studies include process-based LCA studies of Li-ion
batteries with nanomaterials for electrodes, all-solid-state
batteries, batteries with metal anode and lithium metal
polymer (LMP) stationary batteries.12−15
Life cycle assessment (LCA) is a systematic methodology for
investigating and quantifying the potential environmental
Received: November 12, 2018
Revised: January 28, 2019
Published: February 13, 2019

© 2019 American Chemical Society 5082 DOI: 10.1021/acssuschemeng.8b05902

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impacts. As a well-developed method to quantitatively evaluate
the environmental impacts, it has been extensively applied on a
wide range of products and processes. The typical process-
based LCA includes four phases: goal and scope definition, life
cycle inventory analysis (LCI), life cycle impact assessment
(LCIA), and interpretation.9 Process-based LCA has specific
advantage on technology comparison, because it provides
sufficiently detailed information on various types of environ-
mental impacts from each stage of the product’s life cycle.
However, traditional process-based LCA excludes many
upstream processes and suffers from system boundary
truncation.16−18 As a result, the process-based LCA leads to
cutoff errors and the environmental impacts are under-
estimated.18 The EIO-based LCA describes an economy in
terms of financial transactions, inputs and outputs, between
sectors. The system boundary of EIO-based LCA covers the
entire background economy, and it is therefore much more
complete than the process-based LCA.19 Nevertheless, EIO-
based LCA suffers from aggregation error due to aggregation of
industries and commodities, so the accuracy of results from
EIO-based LCA could be sacrificed due to its lower
resolution.17 The integrated hybrid LCA approach combines
the process-based LCA and EIO-based analysis.20 It is widely
adopted to reduce the uncertainty in LCA study. The process
details within system boundary are studied explicitly by
process-based LCA through constructing and analyzing the
detailed life cycle inventory associated with each life cycle
stages within the systems boundary. Besides, the excluded
upstream processes are supplemented by EIO-based LCA to
model and analyze the environmental impacts from back-
ground economy.16,20,21
Most existing Li-ion battery LCA studies focus on the
process-based analysis,22−25 and to the best of our knowledge
no study has conduct to systematically evaluate the “most
comprehensive” life cycle environmental impacts of Li-ion
battery technologies using the integrated hybrid LCA approach
for quantifying both process and EIO environmental impacts.
To fill this knowledge gap, in this work, integrated hybrid LCA
is adopted to study the environmental impacts of two types of
Li-ion batteries with two different cathode materials (NCM
and LMO, respectively) produced in UK. This integrated
hybrid LCA method leverages the advantages of process-based
LCA and EIO-based LCA and overcomes their drawbacks. For
process-based LCA, 17 ReCiPe midpoint environmental
impact indicators and three end point environmental impact
indicators are studied. As for the integrated hybrid LCA study,
life cycle GHG emissions and energy consumption are
considered using available data on life cycle inventory and
EIO data for the U.K. Furthermore, we perform sensitivity
analysis of GHG emissions with respect to the uncertainties in
important factors, including product prices, mass of battery
management system (BMS) and cooling system and
production efficiency. The results provide recommendations
to future development of new Li-ion battery technologies
toward more environmentally sustainable designs. The main
novelty of this work is the comparations between process-
based LCA and integrated hybrid LCA results for Li-ion
batteries.
The rest of this article is organized as follows. In the second
section, materials and methods in this study are introduced,
including overview of integrated hybrid LCA approach, goal
and scope definition, battery technologies, LCI analysis, battery
use phase, end-of-life stage of battery pack, impact assessment
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and life cycle interpretation. The results of process-based LCA,
integrated hybrid LCA and sensitivity analysis are presented in
the third section. A conclusion is given in the last section.
■ MATERIALS AND METHODS
Overview of Integrated Hybrid LCA Approach. The term
hybrid LCA generically refers to any approach that combines process-
based LCA and EIO analysis.21 Hybrid LCA approaches can be
further classified into three types, including tiered hybrid LCA, EIO-
based hybrid LCA, and integrated hybrid LCA according to how the
process-based analysis and EIO-based analysis are combined.18 In
tiered hybrid LCA, process-based analysis and EIO-based analysis are
treated separately.26 Process-based analysis is adopted for the use and
disposal phase and several important upstream processes are also
included in process systems; The remaining input requirements and
LCI are imported from EIO-based analysis.27 The final results of
tiered hybrid LCA can be obtained simply by adding process-based
LCI results and EIO-based LCI results. However, the process systems
and EIO systems are treated separately in this approach, and the
interactions between process systems and EIO systems are not
handled systematically and appropriately. In EIO-based hybrid LCA,
specific commodity sectors are disaggregated from the whole input-
output table to approximate the environmental impacts.28 LCI results
up to the preconsumer stage can be obtained by disaggregating the
whole input-output table; LCI results for the remaining stages of the
life cycle of the product are added to the LCI results up to the
preconsumer stage. Because the EIO-based hybrid LCA approach
partly utilizes the tiered hybrid LCA approach, the interactions
between life cycle stages of the product might not be fully captured in
the analysis results.27 In the integrated hybrid LCA, detailed process
analysis is conducted to estimate the environmental impacts of key life
cycle processes, and the process system is complemented by the
macroeconomic system. The process systems and the macroeconomic
systems are integrated systematically by the upstream and down-
stream cutoff matrices instead of treating them separately in the tiered
hybrid LCA approach. Meanwhile, since process-specific data are
considered more accurate and reliable than the EIO-based data, the
accuracy of analysis is much higher in the integrated hybrid LCA
approach than that in the EIO-based hybrid LCA approach.16,17,29
The mathematical model of integrated hybrid LCA can be expressed
ÅÄÅ A É−1
as follows:17,27,29
− CD ÑÑÑÑ ÄÅÅÅ y ÉÑÑÑ
ÅÅ P
E = [EP , EIO]ÅÅÅ ÑÑ ÅÅ ÑÑ
ÅÅ− CU I − AIO ÑÑÑ ÅÅÅÇ 0 ÑÑÑÖ
ÅÇ ÑÖ
(1)
Here E denotes the total environmental impact, including process
impact and EIO impact. EP and EIO are the environmental extension
vectors of process systems and EIO systems, respectively, representing
the environmental impacts for each process and each economic
sector. The environmental impact data for each process and each
economic sector can be obtained from life cycle inventory data
sources, such as Ecoinvent V3.3.30 AP is the physical flow matrix for
process systems representing physical flows within the process system
boundary, and AIO is the adjusted input-output matrix representing
the interdependencies among industrial sectors within the EIO
systems. AIO is constructed using the EIO data recently reported for
UK. CD and CU are downstream cutoff matrix and upstream cutoff
matrix representing the interactions between process systems and EIO
systems. y is the functional unit column describing the amount of final
products produced per functional unit. The physical flow matrix AP
and downstream cutoff matrix CD are given in physical units. The
adjusted input-output matrix AIO and upstream cutoff matrix CU are
given in monetary units.
Downstream cutoff matrix CD represents flows of goods produced
by process systems to the EIO systems. In this work, compared with
the EIO system for UK, the economic scale of the process system for
Li-ion battery life cycle is relatively small. Therefore, in this work we
treat the downstream cutoff matrix CD as zero. The upstream cutoff
matrix CU represents flows from the EIO systems to the process
DOI: 10.1021/acssuschemeng.8b05902
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Figure 1. System boundary of the process-based LCA for Li-ion battery technologies. Only major components are listed in this figure.

Figure 2. Structure of integrated hybrid LCA model for Li-ion battery, including process systems, EIO systems, downstream cutoff flows, and
upstream cutoff flows.

systems. In order to get CU, we follow the procedures introduced in
the existing literature.31 First, concordance matrix needs to be created
representing correspondence between processes and EIO sectors.
Each sector in the EIO system corresponds to a row and each basic
process is related to a column in the concordance matrix. Matching
sectors and processes are indicated by ones in the matrix and others
are zero. Second, technical coefficient matrix matching process matrix
are created based on the concordance matrix in the first step.
Columns of the upstream matrix CU are populated with technical
coefficients from domestic use and import table. Third, columns of
the matrix from the second step are multiplied with the unit price of
the corresponding basic processes to yield price-weighted coefficients.
After eliminating double counting of the coefficients, we can get the
upstream cutoff matrix CU.

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Goal and Scope Definition. In this work, we conduct process-
based LCA and integrated hybrid LCA studies of two Li-ion battery
technologies, namely LMO battery and NCM battery. For process
systems, a “cradle-to-grave” system boundary is considered which
includes the whole life cycle of Li-ion batteries as shown in Figure 1.
Raw materials extraction, component production, battery manufactur-
ing, use phase and end-of-life stage are considered in this study. For
EIO-LCA part, this study adopts a two-region input-output model
based on supply and use tables for the U.K. and the rest of world
(ROW).31,32
The reasons for choosing the U.K. to illustrate the integrated
hybrid LCA approach are as follows. First, the EIO data recently
reported for UK are sufficient to complement the truncated process
systems, and the data can also reflect the current economic structure
with reasonable accuracy.31 Second, as EIO data only models the
macroeconomic structure and does not account for the specific price
of LIBs, there is always a time delay of several years, before the
economic statistics data are published and the corresponding EIO-
LCA data become available. The newest EIO data for the US in 2015
only contain 71 industries, which are not sufficient to supplement the
process systems, and the EIO data in 2007 with 389 industries may
not accurately reflect the current structure of the economy.33 As the
data become available, the proposed framework can be applied to
other regions and countries, although the present study focuses on the
case of UK. The integrated hybrid LCA approach can evaluate the life
cycle environmental impacts of Li-ion batteries for both process and
EIO environmental impacts. The functional unit is chosen as the
production, use, disposal and recycling of one battery pack.
Accordingly, the life cycle environmental impacts are evaluated
based on this functional unit. The overall structure of the integrated
hybrid LCA approach is illustrated by Figure 2.
Battery Technologies and LCI Analysis. In this work the
environmental impacts of two battery technologies, LMO Li-ion
battery and NCM Li-ion battery, are evaluated. The battery systems
include four main components: battery cell, package, BMS, and
cooling system.
The battery cell consists of five subcomponents: anode, cathode,
cell container, electrolyte and separator.22 For both battery
technologies, anode is composed of a copper current collector with
a coat of negative electrode paste. Synthetic graphite is the main
component of negative electrode, and small amounts of binders are
also included.3,34 The cathode is composed of an aluminum current
collector with a coat of positive electrode paste. The positive electrode
paste consists mainly of the positive active material, small amounts of
carbon black and a binder. For LMO Li-ion battery, the positive active
material is lithium manganese oxide (LiMn2O4); for a NCM Li-ion
battery, the corresponding positive active material is lithium nickel
cobalt manganese oxide (Li(NixCoyMnz)O2). A solvent is applied to
slurry the mixtures in both the positive and negative electrode pastes.
The electrolyte is based on the salt, lithium hexafluorophosphate
(LiPF6), in a mixture of solvents.35,36 The separator is a porous
polyolefin film. The cell container consists of a multilayer pouch and
tabs.
The package for the battery is composed of three subcomponents:
module packaging, battery retention, and battery tray. The BMS
includes battery module boards (BMBs), the integrated battery
interface system (IBIS), fasteners, a high-voltage (HV) system, and a
low-voltage (LV) system. The battery is also equipped with a cooling
system for the purpose of thermal management. An aluminum
radiator is the main component of the cooling system.37 The LMO Li-
ion battery is made with a cathode based on lithium manganese oxide
(LiMn2O4) and an anode based on graphite.23 The NCM Li-ion
battery is made with a cathode based on lithium nickel cobalt
manganese oxide (Li(NixCoyMnz)O2) and a graphite anode.22 The
weight of one battery pack for each type of batteries is considered as
250 kg. LMO Li-ion battery and NCM Li-ion battery share the same
BMS and cooling system technologies.
For LMO Li-ion battery, positive active material lithium manganese
oxide (LiMn2O4) is made from manganese oxide (Mn2O3) and
lithium carbonate (Li2CO3) through several roasting stages in a rotary
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kiln.38 Lithium carbonate (Li2CO3) is made from concentrated
lithium brine with a carbonation step.39 Manganese oxide (Mn2O3) is
produced through a two stage roasting process. For the first stage,
manganese carbonate is roasted in an atmosphere low in oxygen
content; in the second stage, it is roasted in an environment with a
high oxygen content.40 For NCM Li-ion battery, different positive
active materials for cathodes with different ratios of nickel, cobalt, and
manganese are available on the market.41 The ratio of (1:1:1) is
chosen for this study which is used in the literature.42−44 Positive
active material, lithium nickel cobalt manganese oxide (Li-
(Ni1/3Co1/3Mn1/3)O2), is made from lithium hydroxide (LiOH) and
nickel cobalt manganese hydroxide (Ni1/3Co1/3Mn1/3(OH)2).45,46
The production process of metal hydroxides consists in the
precipitation of the metal hydroxides from an aqueous solution of
the metal salts by reaction with a strong base. The products are
recuperated by filtration and dried at low temperature.45,46 The base
materials for the electrolyte of two types of Li-ion batteries include
ethylene carbonate (C3H4O3) and lithium hexafluorophosphate
(LiPF6).47,48 The production of lithium hexafluorophosphate
(LiPF6) uses lithium fluoride (LiF) and phosphorus pentachloride
(PCl5).49
The LCIs of Li-ion batteries are established according to the
process system boundary and functional unit defined in the previous
section. In this study, the process-based LCIs data are built based on
two recent process-based LCA studies for LMO Li-ion battery and
NCM Li-ion battery,22,23 as well as the Ecoinvent database V3.3.30 In
order to make these two types of Li-ion batteries comparable on the
same and fair basis, we update the LCIs both for NCM and LMO Li-
ion batteries. We take the same assumptions from the two recent
process-based LCA studies mentioned previously.22,23,50 In the
existing literature, there are very limited LCA studies both for
NCM and LMO Li-ion batteries. To the best of our knowledge, the
LCA study for LMO battery is probably the only one.23 Besides, both
studies include detailed LCIs data which can be easily referred to and
reproduced to make comparisons with our results. Moreover, these
two studies were published in rigorously peer-reviewed journals,
Journal of Industrial Ecology and Environmental Science& Technology,
respectively, that have been well-recognized by the sustainability
community. Therefore, we choose to build LCIs for NCM and LMO
Li-ion batteries based on these two LCA studies. 22,23 The
compositions of BMS and cooling system are shown in Table 1.
Table 1. Compositions of BMS and Cooling System22
component subcomponent mass (kg)
BMS 9.40 × 100
IBIS 4.50 × 100
IBIS fasteners 3.00 × 10−1
high voltage system 3.20 × 100
low voltage system 1.40 × 100
cooling system 1.00 × 101
radiator 9.10 × 100
manifolds 4.20 × 10−1
clamps and fasteners 2.40 × 10−1
pipe fitting 2.00 × 10−2
thermal pad 2.20 × 10−1
The LCIs of cathode materials of LMO Li-ion battery and NCM Li-
ion battery are shown in Tables 2 and 3, respectively. The LCIs of an
anode are shown in Table 4 and the LCIs of lithium hexafluor-
ophosphate are shown in Table 5. These LCI results include raw
materials, electricity, heat, transportation, infrastructure, and other
related parts for production, use phase, disposal, and recycling of Li-
ion batteries. The processes for raw material inputs cover the
corresponding transportation activities. For the EIO systems, this
study adopts a two-region input-output model based on supply and
use tables for the U.K. and the rest of world (ROW). Specifically, the
resulting adjusted input-output matrix is composed of four parts,
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Table 2. Life Cycle Inventories of Lithium Manganese Table 5. Life Cycle Inventories of Lithium
Oxide Hexafluorophosphate
input unit value note input unit value note
manganese kg 9.18 × 10−1 manganese component23 lithium fluoride kg 1.97 × 10−1 86.7% conversion of
oxide lithium23
lithium kg 2.15 × 10−1 lithium component51 phosphorus kg 1.98 × 100 86.7% conversion of
carbonate pentachloride phosphorus chloride23
oxygen kg 7.15 × 10−1 liquid, for oxidizing hydrogen fluoride kg 4.04 × 100 overspill: 532%23
atmosphere51 nitrogen kg 1.25 × 10−3 liquid, for inert
nitrogen kg 7.86 × 10−1 liquid, for inert atmosphere23 atmosphere22
water kg 3.40 × 100 for suspension: 3 parts water, lime kg 7.44 × 100 neutralization and
1 part Mn2O3 and Li2CO3 disposal of HF22
powder23 electricity kWh 5.39 × 10−1 heat pump24
electricity kWh 5.00 × 10−3 mechanical drive of the rotary electricity kWh 2.00 × 10−3 for pumps, stirring,
kiln23 milling of LiPF623
process heat MJ 1.53 × 101 furnace for rotary kiln23 transport lorry tkm 1.37 × 100 Ecoinvent V3.330
transport lorry tkm 5.64 × 10−1 Ecoinvent V3.330 transport train tkm 8.19 × 100 Ecoinvent V3.330
transport train tkm 3.23 × 100 Ecoinvent V3.330 infrastructure unit 4.00 × 10−10 Ecoinvent V3.330
infrastructure unit 4.00 × 10−10 Ecoinvent V3.330 chemical plant
chemical functional unit
plant
lithium kg 1.00 × 100
functional unit hexafluorophosphate
lithium kg 1.00 × 100
manganese
oxide including the supply and use tables for the U.K. and the supply and
use tables for the rest of the world (ROW). In each table, there are
Table 3. Life Cycle Inventories of Lithium Nickel Cobalt 224 sectors/commodities considered, including the following broad
categories: agriculture, mining, construction, manufacturing, whole-
Manganese Oxide sale trade, retail trade, transportation and warehousing, finance,
input unit value note professional and business services, education and health care, arts and
−1 entertainment, government, and others. The resulting adjusted input−
lithium hydroxide kg 2.50 × 10 lithium component50
output matrix has a dimension of 896 × 896.
nickel sulfate kg 5.42 × 10−1 nickel component22 Battery Use Phase. In battery use phase, Li-ion batteries are
cobalt sulfate kg 5.42 × 10−1 cobalt component22 assumed on an average midsized EV with a weight of 4270 lb and an
manganese sulfate kg 5.23 × 10−1 manganese average driving distance of 200 000 km during a 10-year service
component22 life.52,53 One battery pack is supposed to power the EV on the whole
sodium hydroxide kg 8.36 × 10−1 aqueous solution of lifetime. The driving mix of the vehicle is 55% urban and 45%
metal salts50 highway.54
process heat MJ 5.50 × 10−1 mechanical drive of the End-of-Life of Battery Pack. In existing literature, there are
rotary kiln22
different methods for Li-ion recycling including “recycled-content”
transport lorry tkm 3.67 × 10−1 Ecoinvent V3.330 approach and “avoided burden” approach.55 At the end-of-life stage,
transport train tkm 2.15 × 100 Ecoinvent V3.330 the metal materials in the battery pack are expected to be recycled and
infrastructure chemical unit 4.00 × 10−10 Ecoinvent V3.330 other components of the battery pack are treated as landfill.54 We
plant adopt the “recycled-content” approach in the end-of-life stage of Li-
functional unit ion batteries.56 The main purpose of recycling is material recovery and
lithium nickel cobalt kg 1.00 × 100 the recycling procedures are assumed using current recycling
manganese oxide technologies, including hydrometallurgical and pyrometallurgical
recovery.57,58 In this study, the recovered materials are not treated
Table 4. Life Cycle Inventories of an Anode as raw materials for battery production because materials for battery
production are required to have high quality and purity. The recycling
input unit value note
processes for metal materials are shown in Table 6.
latex kg 1.85 × 10−2 binder50
water kg 4.24 × 10−1 solvent of the binder23 Table 6. Recycling Processes for Metal Materials
graphite kg 4.94 × 10−1 active material22
carbon black kg 1.59 × 10−2 conductive carbon23 material recycling process
copper kg 5.70 × 10−1 negative current collector aluminum hydrometallurgical recovery57
Cu22 copper pyrometallurgical recovery58
sulfuric acid kg 8.08 × 10−2 for treatment of alu foil23 lithium hydrometallurgical recovery57
process heat MJ 1.22 × 100 evaporating water50 cobalt hydrometallurgical recovery57
electricity kWh 2.00 × 10−3 mechanical drive for manganese hydrometallurgical recovery57
pumping slurry50
nickel pyrometallurgical recovery58
transport lorry tkm 1.13 × 10−1 Ecoinvent V3.330
transport train tkm 4.70 × 10−1 Ecoinvent V3.330
Impact Assessment. To evaluate the life cycle environmental
infrastructure unit 4.00 × 10−10 Ecoinvent V3.330
chemical plant impacts of these two battery technologies, life cycle inventory results
functional unit
are converted into corresponding environmental impacts under
different impact categories. Impact categories can be further classified
anode for Li-ion kg 1.00 × 100
battery into midpoint impact categories and end point impact categories.59
Midpoint impact categories can evaluate the direct environmental
impacts, and end point impact categories can estimate the ultimate

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Figure 3. Illustration of midpoint and end point environmental impact categories.
Figure 4. Cradle-to-gate environmental profile for one pack of LMO Li-ion battery.
environmental impacts. Midpoint characterization factors can be
obtained according to equivalency principles, and end point
characterization factors can be obtained by multiplying the midpoint
characterization potentials with the damage characterization factors of
the reference substance.60−62 LCIA methods based on midpoint
categories are midpoint-oriented methods, such as the method
defined in the Handbook of Life Cycle Assessment.9 LCIA methods
based on end point categories are end point-oriented methods, such
as the Eco-indicator 99 and the state-of-the-art ReCiPe methods.63,64
For process system analysis, we choose the end point-oriented
LCIA method, ReCiPe, to quantify the life cycle environmental
impacts of Li-ion battery technologies. For ReCiPe approach, impact
categories and characterization methods are applied to evaluate the
environment profile of Li-ion batteries. There are a total of 17 impact
categories addressed at the midpoint level. These midpoint impact
categories are further aggregated into three end point impact
categories. A total end point environmental impact score can be
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obtained according to the ReCiPe method. Figure 3 illustrates the
relationship between these midpoint and end point impact categories.
For integrated hybrid LCA part, two environmental indicators, life
cycle GHG emissions and energy consumption, are considered. Life
cycle GHG emissions and energy consumption for Li-ion batteries
from process systems and EIO systems are systematically evaluated by
the integrated hybrid LCA method. For life cycle GHG emissions, we
choose the global warming potential (GWP) indicator applying a time
frame of 100 years reported by the Intergovernmental Panel on
Climate Change (IPCC), as a characterization factor for global
warming impact assessment.65 The integrated hybrid LCA ap-
proach66,67 adopted in this study can be applied to other
environmental impact indicators in addition to GHG emissions and
energy consumption, if the corresponding EIO data are available.
Specifically, the environmental impact data corresponding to each
sector in the EIO system are required in the integrated hybrid LCA
approach. However, only GHG emissions and energy consumption
data are available for the case of UK in 224 economic industries.
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Figure 5. Cradle-to-gate environmental profile for one pack of NCM Li-ion battery.
Therefore, we only consider GHG emissions and energy consumption
for the EIO system in this study.
For energy consumption, it refers to the cumulative energy
consumption for the whole life cycle of Li-ion batteries which sums up
various types of primary energies used by each stage for the whole life
cycle of Li-ion batteries. Raw material production, component
assembly, use phase, disposal, and recycling of Li-ion batteries are
considered in this study Energy consumption for the end-of-life stage
of Li-ion batteries consists of the energy consumption for recycling of
metal materials and landfill of other components.
Life Cycle Interpretation. All the results from life cycle impact
assessments will be summarized, and comparison will be made
between LMO Li-ion battery and NCM Li-ion battery. For process-
based LCA, 17 midpoint impact indicators and three end point
impact indicators according to the ReCiPe LCIA method are
addressed. Only cradle-to-gate LCA results are presented for
process-based LCA due to lack of environmental impact data for
battery use phase in 17 midpoint impact indicators and three end
point impact indicators for the ReCiPe LCIA method. For integrated
hybrid LCA, we concentrated on two impact indicators, GHG
emissions and energy consumption. Both cradle-to-gate and cradle-to-
grave LCA results are presented for the integrated hybrid LCA
approach. More insightful suggestions are presented following
sensitivity analysis. For the LCA results, the total environmental
impacts for Li-ion batteries are divided into six parts, including battery
cell, package, BMS, cooling system, disposal and recycling, and EIO
system. Battery cell part includes cell production and pack assembly is
considered in the package part.
To demonstrate the effect of input parameter fluctuations and
quantify the corresponding influences, we perform a sensitivity
analysis by varying input parameters, including mass of BMS and
cooling system, production efficiency and product prices. The results
of sensitivity analysis can insinuate the actual range of error margins.
To further investigate the influence of uncertain parameters on
sustainability indicators, a comprehensive uncertainty analysis based
on Monte Carlo simulation is conducted. The results of Monte Carlo
simulation can show the probability distributions of sustainability
indicators with respect to uncertain parameters.
■ RESULTS AND DISCUSSION
Environmental Profile. Figure 4 and 5 show the cradle-to-
gate environmental profiles of LMO Li-ion battery and NCM
Li-ion battery, respectively. According to ReCiPe LCIA
method, 17 midpoint impact indicators are considered in this
study. For environmental profile analysis, we only consider the
process systems for Li-ion batteries and the EIO systems are
not considered. Each impact indicator is normalized, and the
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total indicator of each category is 100%. From Figure 4, it can
be found that battery cell is the most significant contributor for
13 environmental impact indicators in the environmental
profile of LMO Li-ion battery, including agricultural land
occupation (41.9%), climate change for ecosystems (66.9%),
marine ecotoxicity (90.1%), natural land transformation
(92.9%), terrestrial acidification (66.3%), terrestrial ecotoxicity
(86.1%), climate change for human health (62.5%), human
toxicity (75.8%), ionizing radiation (43.8%), particulate matter
formation (38.4%), photochemical oxidant formation (69.2%),
fossil depletion (57.2%), and metal depletion (84.1%).
Packaging accounts for the largest part in the remaining four
environmental impact indicators, including freshwater ecotox-
icity (42.5%), freshwater eutrophication (45.1%), urban land
occupation (42.9%), and ozone depletion (41.6%).
Battery cell has dominant contributions in 13 environmental
indicators for LMO Li-ion battery. In addition to battery cell,
package also have significant contribution in all environmental
indicators. However, cooling system and BMS only make up
small portions for all environmental indicators.
From Figure 5, it can be found that the NCM Li-ion battery
has an environmental profile similar to that of LMO Li-ion
battery. Battery cell is the most significant contributor for all
the 17 environmental impact indicators in the environmental
profile of NCM Li-ion battery, including agricultural land
occupation (59.7%), climate change for ecosystems (62.4%),
freshwater ecotoxicity (71.7%), freshwater eutrophication
(67.2%), marine ecotoxicity (97.9%), natural land trans-
formation (78.2%), terrestrial acidification (89.3%), terrestrial
ecotoxicity (79.0%), urban land occupation (65.0%), climate
change for human health (62.0%), human toxicity (74.7%),
ionizing radiation (65.0%), ozone depletion (72.0%), partic-
ulate matter formation (82.0%), photochemical oxidant
formation (74.1%), fossil depletion (64.5%), and metal
depletion (83.4%). Battery cell has dominant contribution in
all of the environmental impact indicators, and cooling systems
only makes up a small portion in all environmental indicators
for NCM Li-ion battery. Compared with the environmental
profile of the LMO Li-ion battery, the main difference lies in
the package part. For the NCM Li-ion battery, the package
only makes up a small portion for all environmental impacts,
but it is much more significant in the environmental profile of
the LMO Li-ion battery.
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According to ReCiPe LCIA method, 17 midpoint impact

indicators are aggregated into three end point indicators:
human health, ecosystem quality and resources quality. The
comparison of three end point impact indicators and total
environmental impact between LMO Li-ion battery and NCM
Li-ion battery are provided in Figure 6. The NCM Li-ion

Figure 7. Breakdowns of cradle-to-gate life cycle energy consumption

and life cycle GHG emissions for LMO Li-ion battery.

Figure 6. Comparison between one pack of NCM Li-ion battery and

LMO Li-ion battery in three end point impact indicators and total
environmental impact.

battery is used as the standard for normalization. NCM Li-ion

battery has lower impact in ecosystem quality and resources
quality, but it performs worse in human health. Besides, the
NCM Li-ion battery has a higher total environmental impact
than the LMO Li-ion battery. The most significant difference
lies in the ecosystem impact, where the LMO Li-ion battery Figure 8. Breakdowns of cradle-to-gate life cycle energy consumption
has over 60% higher impact. and life cycle GHG emissions for NCM Li-ion battery.
Integrated Hybrid LCA Results. For the integrated
hybrid LCA of Li-ion batteries, we consider two key 53.9% for LMO Li-ion battery and 55.0% for NCM Li-ion
environmental impact categories, the life cycle GHG emissions battery. EIO systems contribute a relatively small portion of
and energy consumption, in this work, due to the limited around 10% of the life cycle GHG emissions. However, for life
availability of data in environmental extension vectors cycle energy consumption, EIO systems become the most
corresponding to the EIO systems. Different from the tiered significant part, which contributes 49.2% of the life cycle
hybrid LCA approach,68 sectors in the EIO systems are treated energy consumption for LMO Li-ion battery and 47.6% for
in an aggregated way in the integrated hybrid LCA approach. NCM Li-ion battery. Battery cell becomes the second largest
Therefore, we cannot obtain the environmental impacts source of life cycle energy consumption for both Li-ion
corresponding to specific EIO sectors.66,67 To convert the batteries.
GHG emissions into carbon dioxide equivalents, we adopt the Figures 9 and 10 provide the integrated hybrid LCA results
100-year global warming potential (GWP) factors in the fifth for cradle-to-gate life cycle GHG emissions and life cycle
assessment report by IPCC.69 Following the integrated hybrid energy consumption for LMO and NCM Li-ion batteries,
LCA approach, we can calculate both the direct and indirect
life cycle environmental impacts. In Figures 7 and 8, we
summarize the breakdowns of cradle-to-gate life cycle GHG
emissions and life cycle energy consumption of LMO Li-ion
battery and NCM Li-ion battery, respectively. In our research,
we consider 224 economic sectors for the EIO system, and we
focus on the environment impacts of Li-ion batteries. Due to
the large number of economic sectors considered in the EIO
system, explicit listing of sector-level environmental impacts in
the EIO system could not be presented in a clear way.
Therefore, in integrated hybrid LCA results, we treat the EIO
system as a whole and only present the aggregated environ-
mental impacts caused by the entire EIO system instead of
specifying the major environmental impacts by departments
separately. It can be found that the cradle-to-gate life cycle
GHG emissions and life cycle energy consumption have
different breakdowns. For LMO and NCM Li-ion batteries, Figure 9. Integrated hybrid LCA results of cradle-to-gate life cycle
battery cell contributes the most life cycle GHG emissions with GHG emissions for LMO and NCM Li-ion batteries.

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Figure 10. Integrated hybrid LCA results of cradle-to-gate life cycle
energy consumption for LMO and NCM Li-ion batteries.
respectively. For LMO Li-ion battery, the life cycle GHG
emissions is 2336 kg of CO2-equiv per battery pack and life
cycle energy consumption is 58,804 MJ per battery pack,
respectively. For NCM Li-ion battery, the life cycle GHG
emissions is 2126 kg of CO2-equiv per battery pack and life
cycle energy consumption is 59 563 MJ per battery pack. LMO
Li-ion battery has more life cycle GHG emissions and less life
cycle energy consumption than NCM Li-ion battery. However,
the differences in life cycle GHG emissions and energy
consumption between NCM and LMO Li-ion batteries are not
significant. The EIO systems play a key role in evaluating the
life cycle environmental impacts of Li-ion batteries especially in
life cycle energy consumption.
Figures 11 and 12 provide the integrated hybrid LCA results
for cradle-to-grave life cycle GHG emissions and life cycle
Figure 11. Integrated hybrid LCA results of cradle-to-grave GHG
emissions for LMO and NCM Li-ion batteries.
energy consumption for LMO and NCM Li-ion batteries,
respectively. For LMO Li-ion battery, the life cycle GHG
emissions is 25 845 kg of CO2-equiv per battery pack and life
cycle energy consumption is 640 475 MJ per battery pack,
respectively. For NCM Li-ion battery, the life cycle GHG
emissions is 26 452 kg of CO2-equiv per battery pack and life
cycle energy consumption is 655 687 MJ per battery pack. The
NCM Li-ion battery has more life cycle GHG emissions and
life cycle energy consumption than LMO Li-ion battery. The
main reason for higher cradle-to-grave life-cycle GHG
emissions and life cycle energy consumption is that NCM
Li-ion battery contains cobalt and nickel in the cathode part
and the recycling processes of cobalt and nickel have relatively
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Figure 12. Integrated hybrid LCA results of cradle-to-grave life cycle
energy consumption for LMO and NCM Li-ion batteries.
higher environmental impacts compared with recycling
processes of aluminum, copper, lithium and manganese.
Besides, production and processing of these metal materials
also have significant impacts on environment. For cradle-to-
grave life cycle GHG emissions, battery use phase makes up
dominant part both for NCM and LMO Li-ion batteries. It
also accounts for the second largest part in cradle-to-grave life
cycle energy consumption.
Sensitivity Analysis. In order to further quantify the
influences brought about by input parameters, sensitivity
analysis is conducted.70 The results of sensitivity analysis of
LMO Li-ion battery and NCM Li-ion battery in cradle-to-gate
life cycle GHG emissions are presented in Figure 13 and 14,
respectively. The horizonal bars describe the deviations in
cradle-to-gate life cycle GHG emissions associated with
changes in the input parameters. The ranges of each input
parameter are presented on the figures. These two figures
demonstrate that changing input parameters regarding mass of
BMS and cooling system, production efficiency, and product
prices can potentially change the cradle-to-gate life cycle GHG
emissions. The sources of input parameters are shown in Table
7.
From Figure 13 and 14, variations in mass of BMS and
cooling system, as well as production efficiency, have
significant effects on life cycle GHG emissions. We use the
number of battery packs produced in the same plant to
represent production efficiency in this sensitivity analysis.
Larger number of battery packs produced in a plant implies a
higher production efficiency. It is obvious that increasing mass
of BMS and cooling system can lead to higher life cycle GHG
emissions. Higher production efficiency results in lower life
cycle GHG emissions. The upstream cutoff matrix in the
integrated hybrid LCA approach represents commodity flows
in monetary terms from the product sectors in the EIO systems
to the process systems. Therefore, we need price data of EIO
product sectors to construct the upstream cutoff matrix, and
variations in product prices can affect the integrated hybrid
LCA results. Results of sensitivity analysis show that higher
product prices will result in higher life cycle GHG emissions.
However, variations in product prices do not have significant
effects on life cycle GHG emissions. Variations in product
prices can only affect the life cycle GHG emissions from EIO
systems.
It is reasonable to assume that reliable results of the life cycle
GHG emissions are dependent on accurate input parameters.
However, it is not uncommon that fluctuation exists in input
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Figure 13. Sensitivity analysis of LMO Li-ion battery in cradle-to-gate life cycle GHG emissions. The ranges for each input parameter are presented
on the figure while the bars represent the variations in GHG emissions as input parameters are varied from their mean values.

Figure 14. Sensitivity analysis of NCM Li-ion battery in cradle-to-gate life cycle GHG emissions. The ranges for each input parameter are
presented on the figure while the bars represent the variations in GHG emissions as input parameters are varied from their mean values.

Table 7. Ranges, Mean Values, and Sources of Input simulations are conducted using the Oracle Crystal Ball add-in
Parameters for Excel. Each simulation consists of 100 000 Monte Carlo
input parameter unit mean value lower bound upper bound
runs, used to develop GHG emissions probability distributions.
For each run, Crystal Ball randomly selects input parameters
mass of BMS kg 9.40 7.2054 10.8050,54
number of 2.50 × 109 2.20 × 109 50 4.30 × 109 50 based on the predefined probability distributions for four input
battery packs parameters: mass of BMS, mass of cooling system, battery pack
produced per
factory production efficiency and driving distance. Mass of BMS, mass
mass of cooling kg 10.00 7.4071 20.1054 of cooling system, battery pack production efficiency, and
system driving distance are assigned to log-normal distributions.
price of copper EUR 5.52 2.4772 8.9872 The probability distributions of cradle-to-grave GHG
price of EUR 0.005 0.00273 0.00773 emissions for LMO and NCM Li-ion batteries are shown in
manganese ore
price of carbon EUR 0.86 0.6474 0.9974 Figure 15 and 16, respectively. GHG emissions for LMO and
black NCM Li-ion batteries have similar probability distributions.
price of nickel EUR 2.85 2.2875 3.4275 Both probability distributions almost have the same 90%
sulfate
confident intervals, although they have different peak values.
price of EUR 1.44 1.1472 2.4572
aluminum Besides, both probability distributions demonstrate a wide
range of GHG emissions, with the highest bars representing
parameters. Fluctuations in input parameters for Li-ion the values of the highest probabilities. The asymmetric profile
batteries may result from battery production, use phase, of both distributions results from the nonlinear relationship
disposal and recycling processes and estimation in LCI data. between the input parameters and the corresponding
Therefore, several parameters, such as mass of BMS, mass of sustainability indicators. It can be seen that GHG emissions
cooling system, battery pack production efficiency, and driving in both cases are found to be unstable to the presence of
distance exhibit inherent uncertainties in the integrated hybrid
parameter uncertainties. In other words, changes in input
LCA approach. Therefore, probability distributions are applied
to the key input parameters. Simulation methods are further parameters can lead to relatively significant changes in GHG
used to investigate the influence of uncertain parameters on emissions for Li-ion batteries. Therefore, to apply simple and
sustainability indicators introduced above. To simulate the scalable manufacturing methods with less GHG emissions can
probability distribution of cradle-to-grave life cycle GHG lead to more environmentally sustainable Li-ion battery
emissions for LMO and NCM Li-ion batteries, Monte Carlo technologies.
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ACS Sustainable Chemistry & Engineering
Figure 15. Probability distribution of cradle-to-grave GHG emissions for LMO Li-ion battery. The 90% confident region is shown as the blue part.
Figure 16. Probability distribution of cradle-to-grave GHG emissions for NCM Li-ion battery. The 90% confident region is shown as the blue part.
■ CONCLUSION
We evaluated and compared the life cycle environmental
impacts of LMO and NCM Li-ion batteries through process-
based LCA and integrated hybrid LCA approaches. The
integrated hybrid LCA approach emphasized the advantages of
process-based LCA and EIO-based LCA and overcame the
drawbacks of them. The integrated hybrid LCA approach
could estimate the total environmental impacts resulted from
both the process systems and the EIO systems. For process-
based LCA, 17 ReCiPe midpoint environmental impact
indicators and three end point environmental impact indicators
were studied. As for the integrated hybrid LCA, life cycle GHG
emissions, and energy consumption were emphasized.
Furthermore, we performed sensitivity analysis of cradle-to-
gate life cycle GHG emissions with respect to the uncertainties
in mass of BMS and cooling system, product prices, and
production efficiency. Monte Carlo simulations were con-
ducted to simulate the probability distributions of life cycle
GHG emissions for LMO and NCM Li-ion batteries. The
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results of the process-based LCA showed that battery cell
production contributed to the most significant part in most of
the environmental impact indicators. The results of the
integrated hybrid LCA revealed that battery cell production
was the most significant contributor in life cycle GHG
emissions, and the EIO systems contributed the largest part
in life cycle energy consumption. The most significant
difference between two Li-ion batteries lied in the disposal
and recycling stage. For LMO Li-ion battery, disposal and
recycling stage only made up a small portion of less than 10%
for life cycle GHG emissions and energy consumption.
However, for NCM Li-ion battery, it contributed a much
larger part with more than 20%. From the results, we can find
that the EIO systems play a key role in evaluating the life cycle
environmental impacts of Li-ion batteries especially in life cycle
energy consumption. To systematically evaluate the environ-
mental impacts of Li-ion batteries and avoid cutoff errors,
integrated hybrid LCA approach is necessary as the data
become available. Meanwhile, we can figure out the influences
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ACS Sustainable Chemistry & Engineering
of macroeconomic fluctuations on environmental impacts from
results of integrated hybrid LCA approach. However, due to
limited data availability, current integrated hybrid LCA studies
can only analyze some specific environmental impact
categories. As shown by the environmental profiles of two
Li-ion batteries, process-based LCA has specific advantage on
technology comparison, because it provides sufficiently
detailed information on various types of environmental
impacts. Therefore, results from process-based LCA can
make good compensations for integrated hybrid LCA results.
Process-based LCA and integrated hybrid LCA are both
required when evaluating the environmental impacts of Li-ion
batteries. A potential future direction of this research is to
investigate a variety of recycling process and emerging
recycling methods for Li-ion batteries.
■
AUTHOR INFORMATION
Corresponding Author
*(F.Y.) Telephone: (607) 255-1162. Fax: (607) 255-9166. E-
mail: fengqi.you@cornell.edu.
ORCID
Fengqi You: 0000-0001-9609-4299
Notes
The authors declare no competing financial interest.
■
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DOI: 10.1021/acssuschemeng.8b05902
ACS Sustainable Chem. Eng. 2019, 7, 5082−5094