Accepted Manuscript

Material flow analysis on critical raw materials of lithium-ion batteries in China

Jiali Song, Wenyi Yan, Hongbin Cao, Qingbin Song, He Ding, Zheng Lv, Yi Zhang,
Zhi Sun

PII: S0959-6526(19)30093-9
DOI: https://doi.org/10.1016/j.jclepro.2019.01.081
Reference: JCLP 15468

To appear in: Journal of Cleaner Production

Received Date: 26 June 2018

Revised Date: 5 January 2019
Accepted Date: 8 January 2019

Please cite this article as: Song J, Yan W, Cao H, Song Q, Ding H, Lv Z, Zhang Y, Sun Z, Material flow
analysis on critical raw materials of lithium-ion batteries in China, Journal of Cleaner Production (2019),
doi: https://doi.org/10.1016/j.jclepro.2019.01.081.

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Material Flow Analysis on Critical Raw Materials of Lithium-Ion

Batteries in China
Jiali Songa,b , Wenyi Yanb , Hongbin Caoa,b, Qingbin Songc, He Dingb, Zheng Lvd*, Yi Zhanga,b,

Zhi Sunb,*
a
National Engineering Research Center of Distillation Technology, School of Chemical

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Engineering and Technology, Tianjin University, Tianjin 300072, China
b
National Engineering Laboratory for Hydrometallurgical Cleaner Production

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Technology, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190,
China

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c
Macau Environmental Research Institute, Macau University of Science and Technology,
Macau, SAR, 519020, China
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National Development and Reform Commission, Beijing, 100824, China

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*Corresponding author: Zheng Lv (37342272@qq.com); Zhi Sun (sunzhi@ipe.ac.cn)
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National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology
Institute of Process Engineering, Chinese Academy of Sciences
Tel: +86 10 82544844
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Fax: +86 10 82544845

No. 1 Beierjie, Zhongguancun, Haidian District, Beijing, China
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Abstract
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Sustainable growth of the lithium-ion battery (LIB) industry requires a safe supply of raw

materials and proper end-of-life management for products. The lack of research on domestic

critical raw materials and on management systems has limited the formulation of relevant
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policies for LIB-related industries. Here, a critical raw material (CRM) evaluation model was

developed to identify the criticality associated with the supply risk (SR) and economic
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importance (EI) of different materials for the Chinese LIB industry. Dynamic materials flow
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analyses of the relevant critical materials were carried out by integrating a trade-linked model.

Criticality analysis identifies the importance of different materials and optimizes the

subsequent materials flow analysis. The results showed that the in-use stocks share large

portions of material flow for Li, Ni, Co and graphite and further suggests that the market will

not be saturated before 2025. For the end-of-life stage, less than 40 wt.% of the materials in

LIBs can be recycled under the current scheme of materials flow in China; this finding puts

significant pressure on proper waste management. Consequently, it is very important to

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identify effective methods for utilizing the growing amount of waste materials and to provide

a resource supplement for the Chinese LIB industry. This research provides guidelines for

improving management strategies relevant to the critical materials in the LIB industry, for

increasing resource efficiency, and for managing critical resources.

Keywords: Lithium-ion batteries; dynamic material flow analysis; critical raw material;

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Weibull lifetime distribution; China

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1. Introduction

In recent years, the market for lithium-ion batteries (LIBs) has exhibited sustained and rapid

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growth. This growth can be attributed in part to the use of often updated consumer electronics

(CEs), which require high-efficiency batteries (Hu et al., 2018; Zhang et al., 2017).

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Additionally, a large portion of the batteries used in electric vehicles (EVs) and used for grid
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energy storage (GES) have shifted from Ni-MH batteries to LIBs (Peterson et al., 2010). LIBs

have been on the market for less than 3 decades, yet they already dominate the worldwide
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rechargeable battery market with an estimated 85% market share (excluding lead-acid

batteries) (Pillot, 2015). China has become the largest LIB manufacturer, accounting for more
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than 50% of the market share with a production of 63.7 GWh in 2016 (CHYXX, 2017; Wang
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et al., 2017) (Fig. 1).

80 Energy storage in China

Production amount of LIBs, GWh

Electric vehicles in China

Consumer electronics in China
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70
Rest of the world, all applications
60

50
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40
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30

20

10

0
2011 2012 2013 2014 2015 2016 2017
Year
Fig. 1 Lithium-ion battery production amount in China and the world

The rapid development of the LIB industry has attracted global attention to associated
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environmental and resource problems. As one of the most important types of new electronic

waste (e-waste), LIBs contain many potentially hazardous materials, including heavy metals

and organic chemicals. Improper disposal will cause severe environmental problems (Liang et

al., 2017). Moreover, e-waste containing LIBs has been classified as hazardous waste in many

countries due to its high flammability (Grant et al., 2013). LIB production continues to

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increase rapidly while an effective recovery system is undeveloped. The large consumption of

valuable materials (Li, Ni, Co, graphite, etc.) for LIBs has imposed significant pressure on

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worldwide suppliers, accounting for 50-70% of the total cost of LIBs (Gu et al., 2017). Across

all applications, LIBs account for the greatest share of Li (75% in China and 46% worldwide,

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2016) and Co consumption (76.6% in China and 44% worldwide) (CHYXX, 2016; USGS,

2018). Mining efforts for these valuable resources has increased at a considerable rate, while

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the recovery volume of secondary resources does not occur at the same level. For example,
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Co mining production in the U.S. increased by 4.75 times from 2014 to 2016, while the

recovery volume of secondary resources only increased by 0.23 times (USGS, 2017). Thus,
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the international community should focus its concern on the supply safety and environmental

sustainability of LIB resources (Allwood et al., 2011; Helbig et al., 2018).

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Driven by the appeal of sustainable development and environmental protection, attention has
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been paid to the potential risks during the resource life cycle. To trace the material

metabolism in a specific spatial frame and time horizon, several studies have employed
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material flow analysis (MFA) as an approach to analysing material qualities, locations and

cycles in the anthroposphere. Using this method, the overall picture for essential resource or
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material flows in cities (Ibrahim et al., 2013; Song et al., 2016), countries (Lu et al., 2017;

Swain et al., 2015), and even the whole world (Liu and Muller, 2013; Ongondo et al., 2011)
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can be observed. MFA can provide valuable insights into recovery rate quantification,

emissions, loss assessment, and international trade estimation, especially for metals (Chen

and Graedel, 2012). MFA is a decision-support tool for policymakers and environmental

managers, both in the resource and waste management fields. Current publications on LIB

element flows and their major findings are summarized in Table S1. Among the materials

used in LIBs, the material/substance flows of Li (Lu et al., 2017; Sun, X. et al., 2017; Weil et

al., 2009; Ziemann et al., 2018), Co (Sommer et al., 2015; Zeng and Li, 2015) and Ni (Huang
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et al., 2014; Zeng et al., 2017) have provided some insights on the material flows for products

using these elements. However, current MFA studies usually only examine one kind of metal

element from LIBs, and few MFA models have been used to analyse the differences and

connections of multiple materials in one application (Vaalma et al., 2018; Weil et al., 2018).

When one material is used in many applications, the researchers have to dedicate a significant

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portion of their effort to discussing material flows in fields other than their primary focus.

Meanwhile, the selection of key materials for LIBs was based on descriptive rather than

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calculated methods. Furthermore, few studies examined international trade flows across the

whole life cycle of the various materials, failing to include materials that are imported or

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exported along with that of the electronic products. Such analyses may be difficult because

data on different flows are not uniform, and data sources contain contradictory information.

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To fill these gaps and create a customized MFA for LIBs critical material flows on a country
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scale, we present a new CRM-MFA model established by combining a critical raw materials

(CRMs) evaluation and a dynamic MFA. Sorting trends for the critical materials used in the
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LIB industry were identified. The analysis was constrained to China and focused only on the

LIB sector. Flows and stocks for selected CRMs were estimated and compiled across the
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entire life cycle. Variations in the flow and stock of materials was traced over technological
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upgrades. Based on these calculations and analyses, it was possible to identify the bottlenecks

and barriers that hinder sustainable development of the LIB industry. The results of this study
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suggest ways to foster a sustainable supply of materials for national or international markets,

to boost the efficiency of resource use, and to support a future waste management system
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(Weil et al., 2018).

2. Methodology
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2.1 System boundary definition

The goal of an MFA is to increase the understanding of a system defined by spatial and

temporal boundaries. In this study, a material boundary was also introduced into the model to

account for the primary flows in one specific sector. Based on the cost and the mass

constitution of LIBs, we focused primarily on the cathode and anode materials in LIBs to

calculate the relative criticality of the raw materials. For cathode materials, we examined the

non-layered LiFePO4 (LFP), including both Li and Fe, and layered LiMO2, where M could be
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one or more of the following elements: Ni, Co, Mn and Al. For anode materials, graphite

carbon, Cu and Ti were also investigated (Nitta et al., 2015). These 9 raw materials were

simultaneously examined to determine the CRMs. Note that the metals in battery shells and

packs were not considered in this paper.

Since China has played a key role in both LIB production and recovery, this study defined the

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spatial boundary as the anthropogenic cycle of several selected CRM flows on the Chinese

mainland (excluding Hong Kong, Macau and Taiwan). The temporal boundary was defined as

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the time period from 2010 to 2016 because the global EVs market experienced a significant

surge during this time (Fig. 1). Since the advent of smartphones in 2011, the Chinese

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smartphone industry has entered a period of vigorous development; 2013 was used as the

representative year for this new era of CEs. With the promulgation of the ‘Energy Saving and

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New Energy Vehicle Industry Development Plan (2012-2020)’ in China, the application of
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LIBs in EVs also entered a new era. Thus, the years 2013 and 2016 were chosen to reflect the

trend in critical flows driven by these market changes in China. To the extent possible, the
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reference period for the data used in the criticality assessments was based on the latest 4-year

average (i.e., 2013-2016).

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The life span of LIB materials can be divided into 5 stages: critical raw materials preparation,
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LIB production, product fabrication, consumption of in-use stock, and waste management

(include recovery and reuse). All of these stages play a significant role in describing material
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flows. Detailed start and end points of these stages are marked in Fig. 2. Each life stage

contains subcategories. For example, the raw materials preparation stage refers to physical
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changes that occur during refining such as the chemical transformation of lithium to lithium

carbonate, lithium hydroxide, or lithium chloride. The import/export of waste during the
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waste management stage for all four materials was not included here due to a paucity of data.

LIBs are listed as Class 9 Miscellaneous hazardous materials, and the State Council of China

has formulated several policies to limit the import of solid wastes, including EoL batteries

(State Council, PRC, 2017). Therefore, the customs department does not include any relevant

statistics about illegal trade.

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International Market
FI1 FO1 FI2 FO2 FI3 FO3 FI4

MxOy
Mx(OH)y LFP-C
Critical Raw NCM-C CEs
Mineral Mx(SO4)y LIBs Products Consumption
Materials LCO-C EVs
/Brine
F'M Preparation FM
Mx(CO3)y F'P Production FP LMO-C F'E
Assembly FE FU
In-use Stock
GES
MxCly ……
FL1 …… FL2 FL3 FL4
FR2

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FC
Waste Management
(Recycle / Reuse)

FL5
FR1

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System Boundary National Market

Material Trade Flows

Products Trade Flows Transformation Flows Loss Flows Recovery Flows

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Fig. 2. Lithium-ion battery life cycle and system boundaries

2.2 Criticality evaluation factors

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CRMs are not only essential for the production of goods powered by LIBs in everyday use
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but also for the national development of eco-efficient and globally competitive technologies.

Therefore, a top priority is to identify factors that can be used to evaluate the extent to which
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one material influences the LIB industry and market. Generally, these factors include the

resource value, constituents of the products, how indispensable a resource is in production,

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the risks to supply sustainably, etc. Economic importance (EI) was used as a measure of a
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material’s importance in a specific economy through end-use applications and the value added

(VA) of corresponding sectors. Supply risk (SR) was defined to reflect the severity of the
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impact on disruption of supply chains and was based on the concentration of major suppliers

and governance security. The model used to assess EI was derived in accordance to the model
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developed by the European Commission research group (EC, 2017). However, we focused
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only on China and the LIB sector, so the influencing factors selected herein were those

relevant for Chinese national conditions, and some of the parameters from the European

model were redesigned, e.g., the trade reliance ratio.

The economic importance of M in the LIB industry ( EI M , LIB ) was calculated as the

weighted sum of the gross VA of end-use sectors that consume M . When multiplied by the

material cost share of LIBs, this parameter can be used to characterize the economic impact of

a sudden break in supply affecting LIB industries as follows:

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1 s
EI M , LIB =y M
GDP
∑ ( xM ,s As SI M ,s ) (1)

where M indicates the raw material/metal used in LIBs; y M is the share of M cost in the

LIB industry; xM , s is the share of raw material demand from sector s; As is the value of

the corresponding using megasector; and SI M , s is the substitutability of M in sector s.

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s
Note that ∑x M ,s = 1 was encompassed for all applications of the raw materials.

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The risks to M in the supply chain were caused by several factors: lack of substitutes, low

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recovery rates, high concentration and poor governance in primary production countries.

These four elements were brought together into a single indicator, i.e.:

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SRM , LIB =SI M TRM (1 − ρM ) HHIWGI , M (2)
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where SI M accounts for the substitutability of M in the LIB industry, ρ M is the fraction

of demand that is met by recovered materials, and HHIWGI , M characterizes the concentration
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of production and the governance status at the country level, i.e.:

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HHIWGI ,M = ∑ ( Sc2WGI c ) (3)

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Here WGI c is the World Governance Indicators of country c ; and S c is the fraction of

worldwide production in country c . This provides the basis for calculating the SR due to
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poor governance.

TRM indicates the trade reliance ratio:

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D o+ Im − Ex
(4)
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TRM =
Do
where Do presents the domestic production amount of M , Im presents the import

amount and Ex presents the export amount. D o+ Im − E x is the domestic LIB production

demand of M , If the domestic production can satisfy the domestic demand, TRM ≤ 1 . If not,

the resource needs to rely on the import, then TRM＞1 .

2.3 Establishment of the CRM-MFA model

To build a new model to quantitatively evaluate the management system for the life cycle of
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LIB materials, this study proposes a method constrained to the Chinese LIB industry. The

definition of raw material criticality is summarized as follows:

Criticality=Supply Risk ⋅ Economic Importance (5)

A criticality matrix was used to normalize and project the raw materials into a uniform matrix

with contour lines (Glöser et al., 2015). The products of the two normalized indicators (SR·EI)

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were used to rank the criticality for quantitative comparisons (Helbig et al., 2016).

Among the 5 stages of the LIB life cycle, the consumption stage is considered to be the only

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process that stores materials, so stocks in production or recycling factories could be neglected;

the flow from raw materials to the final product was regarded as a continuous process. A static

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approach was applied to assess the material flows in the abovementioned stages (Fig. 3a).

However, for the consumption process, products often stay in service for several years, and a

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few products would be considered stock after ending their life, so it is difficult to describe the
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amount of product entering the next stage. Hence, a dynamic top-down approach was used to

describe the waste entering into the waste management route (Fig. 3b). In this study, idle or
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in-use stocks were regarded as a whole because they both stay in consumers’ hands before

going onto subsequent stages.

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Fig. 3. Material flow model of a unit as a static process (a) or a consumption process (b) with

in-use stock
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Based on the principles of MFA, calculations describing each process should obey the mass

conservation law (Muller et al., 2014). Here, flows from one process to the next process,

losses to the environment, and exchange with the international market were considered. The

accumulations of stock from different reservoirs were identified in a dynamic process. Eq. (6)

shows the calculation method of in-use stock. Stocks and flows were modeled at a time series

t , typically ∆t = 1 year in this research.

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T
S [T ] = S [0] + ∑ ( FI [t ] − FO [t ]) (6)

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t =1

T T N

∑ ( FI [t ] − FO [t ]) = ∑ ∑ ( Pn, I [t ] ⋅ cn, I [t ] − Pn,O [t ] ⋅ cn ,O [t ]) (7)

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t =1 t =1 n =1

where S [T ] is the in-use stock at a time T ; S[0] is the initial value of the first invested

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year; FI (t ) is the material inflow; FO (t ) is the material outflow; Pn presents the
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different LIB products; c n presents the material concentration in the products; N is the
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total number of the LIB types considered, which is 4 in this research.

For the material inflows, a rich set of historical data is accessible from the production process.
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However, there are different methodologies to quantify the outflows, including population
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balance model (Hatayama et al., 2007; Yokota et al., 2003), logistic survival model (Cheah et

al., 2009), delay model (Kleijn et al., 2000), and etc. The waste LIBs generated annually can

be calculated based on the changes in the lifespan functions f (T ) with time series input t .
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This approach is called population balance model or residence time model, which can be
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mathematically described as Eq. (8):

Tmax
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FO [t ] = ∑ ( f (T ) ⋅ FI [t − T ]) (8)
T =1

where FO [t ] is the annual output of EoL LIBs, FI [t -T ] is the amount of LIBs flowing into

the consumption process in (t -T ) year, and f (T ) is the probability densities of waste

scraps arising in the year t with a battery lifetime of T . Weibull lifetime distribution ,

which can assume a wide variety of shapes to apply for more situations (Song, X. et al., 2017),

was used as lifetime distribution functions f (T ) in this study. The function was given as Eqs.
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(S1)-(S3) in the supplementary materials, where T represents service life (calendar

lifetime), which is a simplification of the model. The calendar lifetime of LIBs was

determined by both the cycle lifetime and using frequency.

2.4 Data collection and sources

To ensure the robustness and comparability of the results and maximize the quality of the

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outputs of the study, the availability and quality of the data in this study should be guaranteed.

It should be noted that the data of EC were not calculated for LIBs industry particularly, and

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some import/export data or recycling information were not suitable for Chinese situation. So

based on the CRMs data of EC (EC, 2017), the revised criticality methodology also combined

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with official Chinese data over that from trade/industry associations, other special interest

groups and best estimation. Besides a detailed literature review, stakeholder consultations

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were also carried out, including the major LIB manufacturers, recycling companies, official
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management agencies in China.

Different flows were calculated in 3 different ways depending on the data availability:
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directly based on existing data, derivation from existing data, and reasonable assumption

based on MFA principles. As the data sources are various, the priority order of data sources in
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this study is Chinese official data (e.g. National Bureau of Statistic (NBS) and General
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Administration of Customs (GAC)), data published in the authoritative journals, data for

China over global datasets (e.g. the United States Geological Survey (USGS) and European
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Commission (EC)), some trade associations or non-official organizations’ data from

industry/market research in China after checking reasonable, some questionnaire survey, best
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estimation or expert judgment. This sequence also reflects the sensitivity coefficients.

All data in section 3 have been checked by mass balance. The results should in accord with
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the official estimates and the situation of Chinese LIB industry, which tends to verify the

accuracy of estimates for some missing data. The main data sources in this study are shown in

Table 1.

Table 1

Data sources used in this study

Process Data type Data sources
Input & Export All material China Customs Statistics Yearbook (2014-2017)
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USGS, National statistical data provided by the
Mineral
CNMIA (2014-2017)
Battery grade
Calculated according to the mass balance
Domestic chemicals
production Yearbook of Electric Power Industry in China
LIBs
(2014)
Yearbook of the People's Republic of China
CEs & EVs
(2014-2017)

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Calculated by upstream with Weibull lifetime
In-use stock Selected material
distribution equation
Waste in productive

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(Song, J. et al., 2017)
process
Loss
Waste in consumption
(Zeng et al., 2015)

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process
Waste Collection efficiency (Richa et al., 2017; Song, X. et al., 2017)
management Recovery efficiency (Li et al., 2017)

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3. Results and discussion

3.1 Criticality analysis

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The criticality evaluation factors SR and EI of 9 raw materials in Chinese LIB industry were

calculated using the average data from 2013 to 2016. Detailed parameters and calculations
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can be seen in Tables S2 and S3. After normalization and projection, the raw materials were
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plotted into a uniform matrix (Fig. 4). Calculation principles and detailed processes for the

criticality evaluation are shown in Fig. S1 a-c.

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Fig. 4. Normalized SR*EI matrix and criticality evaluation results for 9 materials contained in

lithium-ion batteries using average data from 2013 to 2016.

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Based on the normalization and projection results, two contour lines were identified between

the material locations. Where the dots are far from the ‘X’ and ‘Y’ axes (SR·EI≥12), the

criticality was determined to be high (as shown in the red and orange areas of Fig. S1b).

Similarly, materials with 3<SR·EI<12 were designated as medium-high criticality (deep

yellow area of Fig. S1b). The dots with (SR·EI≤3) represent the non-critical raw materials

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(green area of Fig. S1b), which have little effect on the LIB industry. The thresholds values (3

and 12) separating the various zones in Fig. S1b were selected based on comprehensive

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consideration of element location and matrix partitioning. Resilience scores of approximately

20% below the medium-high SR·EI curve and above the high SR·EI curve were set to avoid

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problems with underestimating a material’s criticality. The final results of the CRM

evaluation are shown in Fig. 4. CRMs for LIBs were classified and highlighted by blue dots

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in the criticality zone. Based on these results, we chose 4 materials (Li and Co with high
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criticality; Ni and graphite with medium-high criticality) as critical materials for analysing

flows in China. We analysed every process during the life cycle of each critical element in
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detail and discussed the bottleneck issues.

3.2 Process analysis of CRM-MFA

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3.2.1 Raw material mining and preparation

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Fig. 5. Global distribution of lithium-ion battery critical material reserves. Note: the length of

the bar indicates the relative fraction of the total reserves.

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Generally, the flow of raw materials in the economy starts with mineral extraction. At the

resource mining stage, there are 3 kinds of resources: ore, brine and secondary resources. A
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global overview of critical metal reserves needed for LIB production is shown in Fig. 5 (the
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data pertains to resources that can be economically extracted at the time of reporting).

Reserves of raw material commodities are dominated by a few countries, with three countries
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providing 90.7% of Li, 70% of Co, 46.9% of Ni, and 86.8% of graphite resources. The global

supply chain of critical resources could breakdown suddenly due to economic or political
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instability in these primary suppliers. The bar chart in Fig. S2 depicts the resource availability

of 5 major LIB materials in China. Although China is one of the top three countries with Li
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and graphite reserves, TR of critical materials such as Li, Co, Ni all rely on imports, with

more than 80% of the supply coming from outside China. Due to the particularity of Li brine

resources in China, there are difficulties with Li extraction in China. Even though Li brine

accounts for 78% of the Li reserve in China, more than 90% of domestic production comes

from Li ore. Thus, China relies heavily on imports to meet Li demand. The high reliance on

the import of raw materials needed for cathode production is a potential threat to resource

security for LIB industries in China.

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After mining, metal minerals are converted to basic chemicals for LIB production, i.e., metal

carbonate, metal hydroxide, and metal chloride. More details on the import and export of the

four critical resources are given in Table S4.

3.2.2 LIB production

Commercially, cathode materials vary significantly, while graphite is typically used as the

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anode. The value chain for LIBs is therefore influenced by the supply of a series of basic

chemicals. For example, lithium carbonate is used as a raw material to produce derivative

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materials, i.e., LiCoO2 (LCO), LiMnO2 (LMO), LiNixMnyCo1-x-yO2 (NCM), LiNixCoyAl1-x-yO2

(NCA). Fig. S3 shows major innovations in material technology for past, current and

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expected battery chemistries. From the earlier LMO, LCO, and LFP to the current NCM/NCA

and even Li4Ti5O12 (LTO) batteries, LIB materials have been continuously updated to meet

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demands. The use of cheaper materials is the trend for the future. High-priced and scarce Co
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will gradually be replaced by cheap available metals such as Ni or Mn, and even other

nonmetals such as air or sulphur. Fig. 6 shows the estimated amount of production of the 4
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main cathode materials in China from 2013-2016. Typical compositions of the four LIB types

are shown in Table S5. Combined with production and composition data, it is easy to
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determine the critical resource consumption from 2013 to 2016. As producers have churned
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out ever more LIBs, the production of LFP and NCM has grown rapidly, while increases in

the outputs of LCO and LMO have not been obvious. To control cost and alleviate shortages
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of Co resources, mixed metal materials have gradually replaced LCO, exhibiting a trend of

"high Ni and low Co". NCM333, NCM523, NCM622 and NCM811/NCA accounted for 13%,
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76%, 10% and 1% in 2016, respectively. This change has saved 48.4 wt.% consumption of Co

resources annually and effectively relieved pressures due to resource deficiencies.

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Fig. 6. Production amount of 4 prototypical cathode materials in China from 2013 to 2016

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3.2.3 Product assembly

It is easy to determine material flows classified by chemical composition using existing data,

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but there are not yet systematic and through descriptions of flows for specific applications in
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China (Yi et al., 2018). The balance between LIBs and final products were assessed using

MFA. Various products are powered by LIBs, including CEs, EVs and GES systems. With the
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development of technology, a great variety of CEs were created: mobile phones, laptop

computers, digital cameras and so on. EVs can be further divided into hybrid electric vehicles
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(HEVs), plug-in hybrid vehicles (PHEVs), and battery electric vehicles (BEVs). While some
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HEVs use Ni metal hydride batteries, LIBs are more attractive for PHEVs and BEVs. In

addition, the scale of the electric bicycle market in China cannot be ignored. Detailed
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characteristic of typical LIB-powered devices and applications are summarized in Table 2.

Approximately 65.8 wt.% of LIBs in China were used in EVs applications; this proportion
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was driven by the large mass of EV batteries and increases in production capacity. Allowing

for 20% omission of devices, approximate 457.9 kt of LIBs were assembled for use in various
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products and then went into consumption. In addition, we anticipate that approximately 224.3

kt (32.8 wt.%) of LIBs were sold directly to consumers to replace old batteries without these

batteries going through the product assembly process.

Table 2

LIB-powered device characteristics (Gruber et al., 2011; Hao et al., 2017; Sun, Z. et al., 2017;

Winslow et al., 2018).

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Anticipated Approximate
Typical LIB Production
LIBs total
mass range amount in
Sub-type lifespan in consumption Import amount Export amount
Application in different China,
application the of LIBs, of China,2016 of China, 2016
products 2016
application 2016 (metric
(kg) (units)
(years) tons)
2100 46.2 billion 126 billion
Mobile phone Mobile phone 3 0.02-0.04 63,000
million USD USD
Laptop 5.5 0.18-0.47 170 million 55,250 23.6 billion 182 billion
Computer
Tablet 5.1 0.03-0.1 80 million 5,200 USD USD

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Digital Digital 15.3 25.2 million
6.5 0.06-0.16 1,680 -
camera camera million units
421.8
BEV 8 180-400 122,330

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thousand
93.9 15.2 thousand 31.3 thousand
EVs PHEV 8 100-280 17,840
thousand units units

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Electric
5 5.2-15.0 10 million 101,000
bicycle

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It is also possible to identify split-flows for Li, Co, Ni and graphite when LIBs are assembled
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into products. The emergence of mixed metal materials has changed the applications of CEs

and EVs (Fig. 7). NCM/NCA gradually replaced some portion of LCO used in CEs and LFP
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used in EVs. For the past 3-5 years, LCO has held a dominant position in the CE market

because of its superb energy density, which enabled production of thinner electronic
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equipment. Along with progress in research and development, high Co prices made some
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manufacturers choose alternative NCM/NCA products with similar performance. Furthermore,

LFP may be replaced by layered cathodes because of higher energy density requirements.

LMO is also being phased out of the rapidly developing market due to its instability. In GES
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applications, LFP may continue to play a role because of cost considerations and the orderly

recovery of spent LIBs from EVs.

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LCO LFP NCM/NCA LMO Other
100

Percentage (kWh/kWh,%)
80

60

40

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20

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0
CEs CEs EVs EVs GES GES
2013 2016 2013 2016 2013 2016
Applications, Year

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Fig. 7. Changes in cathode types for the top three lithium-ion battery applications in China

from 2013 to 2016

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3.2.4 Consumption and in-use stock

After the three steps described above, materials eventually reach the consumer. As mentioned
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in Section 3.2.3, batteries for different products have a distinct service life. However, for

practical use, the designed service life is often reduced by many factors. For example, when
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the battery capacity of a new energy vehicle is less than 80%, it will be scrapped (Richa et al.,
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2017). In China, LIBs used in EVs are used with high frequencies, e.g., in taxis or electric

bicycles, which leads to a significant reduction in battery lifetime. It is important that LIBs,
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especially in CEs, are reserved somewhere by consumers at the end of their service life rather

than becoming part of the output flow (Daigo et al., 2007). Taking into account “hibernating”
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materials maintained by consumers and the anticipated lifespan of the LIBs in typical devices

(shown in Table 2), this study assumed an average residence time for the LIBs used in CEs,
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EVs, and GES of 3, 5, and 7 years in low lifetime scenario, and 5, 7, and 10 years in high
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lifetime scenario, respectively. The Weibull lifetime distribution functions of LIBs under 3

lifetime scenarios can be found in Fig. S4a-c. The dynamic MFA model was used to calculate

the storage accumulation and output waste generated during the consumption process. This

calculation either retrospectively determined stocks and flows based on historical data or

predicted the future scrapped amount by extrapolation. Using Eq. (4) - (8), the annual LIB

cathode waste generated in China from 2012 to 2017 can be estimated.

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generation in China (thousand metric tons)

400 Low lifetime scenario

Annual waste LIBs cathode material

350 Baseline scenario
High lifetime scenario
300
Baseline scenario
250 LFP
NCM/NCA
200 LCO
LMO
150

100

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50

0
2012 2014 2016 2018 2020 2022 2024

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Year

Fig. 8. Estimation and forecast of changes in lithium-ion battery waste flows from 2012 to

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the future. Note: the bar chart is based on the baseline scenario.

The generation of LIB waste keeps increasing year by year, and this situation has been

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extremely serious since 2013 (Fig. 8). Based on the model predictions of production, the
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amount of cathode scrap was forecasted to be 89.20-133.54 kt/a in 2020 and 275.01-391.83

kt/a in 2025. Under the baseline scenario, there will be 108.06 kt/a and 327.70 kt/a cathode
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scrap generated in 2020 and 2025, respectively. The growth rates of both LFP and NCM/NCA

are decreasing (Fig. S5), and the period of explosive growth is nearing completion.
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NCM/NCA was predicted to be the fastest growing waste stream of cathode materials after
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2018.
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Fig. 9. (a) Annual incremental changes in the amount of cathode materials in storage from

2013 to 2016 under a low lifetime scenario and high lifetime scenario compared with the

amount in production. (b) Annual calculations and predictions of the amount of cathode

materials in storage from 2013 to 2025 under the baseline scenario.

Notably, materials stored during the consumption process exhibited a multi-fold increase. The

amount of LIB cathode materials stored during the consumption process increased from
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300.62 to 366.79 kt between 2013 and 2016 (Fig. 9a). According to the baseline scenario

(shown in Fig. 9b), LMO and LCO stocks will become saturated in 2025, and LFP is reaching

the saturation point. LIB markets in China will not be saturated in 2025 because EVs are

becoming ubiquitous and GES are being used more generally. High efficiency management of

e-waste is becoming a problem that requires greater attention.

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3.2.5 Waste management

There are three potential streams for the treatment of spent LIBs: product reuse, material

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recovery, and waste disposal. It was estimated that the collection rate of spent LIBs was at an

extremely low level worldwide. The collection rate of spent LIBs was 45% in the EU but

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lower than 40% in China (Knights and Saloojee, 2015). Most parts of the spent LIBs were

discard in the environment, with no chance to flow into the waste management process. To

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meet the growing resource demands, an integrated waste management system should be
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established in the future. Reuse and recycling are considered as the risk-reducing measures

for the collected spent LIBs. With the aim of maintaining resources sustainability and
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reducing the environmental impact of spent batteries, many effective methods were applied to

cope with the spent LIBs. The processes of frequently-used treatment approach, namely
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pyrometallurgical, hydrometallurgical, pyrometallurgical + hydrometallurgical, and other

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methods (e.g., ultrasonic, mechanical) (Fig. S6a). The Chinese government has certified 109

formal e-waste enterprises for dismantling 100 million waste home appliances per year,
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including the dismantling of spent LIBs. Some companies recycle LIBs on a commercial

scale (e.g., GEM, Haopeng, Bangpu), industry infrastructure had progressed a lot from
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2013-2016. Through the investigation of the known recovery enterprises, approximate

treatment capacity and recovery rate are shown in Fig. S6b and S6c. Currently,
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hydrometallurgical, pyrometallurgical, and combination of them are the commonly accepted

methods in industry. The recovery rate of each method improved fast in recent years. Current

recovery efforts are focused on cathode materials because of their high contribution to the

total battery mass, cost, and use of critical metals. Although graphite is often used for internal

energy gain, the production of graphite has typically corresponded with large amounts of

waste water emissions. It is therefore important to consider graphite recycling especially in

areas with less primary production. The emergence of synthetic graphite and LTO materials is
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a result of pressure related to performance requirements and the paucity of graphite recovery.

Recovery would be a way to decrease natural graphite dissipation and achieve comparable

performance.

3.3 Evaluation of the life cycle of different critical materials

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Fig. 10. Sankey diagram of material flows in the Chinese lithium-ion battery economy in
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2016: (a) Li, (b) Co, (c) Ni, (d) graphite. Note: Waste generation is based on the baseline

scenario. Among the flows in product assemblies, 32.8 wt.% of materials flowed into
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consumption directly as replacement batteries without going through the production process.

The flow diagrams only present final applications.

Mass balances of critical materials in Chinese LIB industries are examined and summarized

in Fig. 10. In 2013, the critical resource consumptions during LIB production were 4 kt Li,

25.5 kt Co,7.7 kt Ni, and 54.7 kt, while in 2016, consumptions were 9.5 kt Li, 38.4 kt Co,16.7

kt Ni, and 122.6 kt graphite (Fig. S7).

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Li is a core component for each type of LIB. Of the total Li used for LIBs, 29.5 wt.% is in

LCO, 8.1 wt.% in LMO, 21.3 wt.% in NCM/NCA, and 41.1 wt.% in LFP. Over-reliance on

imports is one of the major problems in China, and 86.5 wt.% of Li resources are imported

(Fig. 10a). Although Li resources, both in China and worldwide, are predominantly found in

brine, imports and domestic production of raw minerals primarily depend on ore. Moreover,

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although Li ranks as the most important element in the criticality evaluation, the recovery rate

of Li during the recycling process is less than that of Co and Ni because of the low content

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and high cost. This situation is very unfavourable for balancing resource supply chains and

achieving a closed-loop process.

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Co is currently the most valuable component of LIBs. However, Co resources in China are

scarce, and 89.0 wt.% of Co comes from imports (Fig. 10b). Co is mainly used in production

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of LCO and NCM/NCA batteries. To save costs but provide similar performance, Co in LIBs
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has gradually been replaced by Ni, Mn, and Al, all with a lower price point. The use of Co as

LCO has decreased from 71.1 wt% in 2013 to 59.8 wt.% in 2016.
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Ni is primarily used in NCM/NCA (98.1 wt.%) batteries because LiNiO2 batteries have been

phased out of the market. Although 62.2 wt.% of Ni resources come from imports, LIBs only
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account for a small percent of Ni use. It is now critical to develop production methods for Ni
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derivatives using domestic raw materials in order to reduce imports of high value-added raw

materials.
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Graphite is widely used in production of all types of battery materials, with 25.4 wt.% using

in LCO, 18.1 wt.% in LMO, 21.9 wt.% in NCM/NCA, and 34.6 wt.% in LFP. Here, graphite
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was representative of anode materials, and the material flow of graphite has changed over

time. With the development of anode materials, LTO and higher performance artificial
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graphite have gradually replaced non-renewable natural graphite resources, shifting from 50%

natural graphite and 48% artificial graphite in 2013 to 36% natural graphite, 53% artificial

graphite, and 11% mesocarbon microbeads in 2016. China is the largest producer of graphite

in the world and as such can fully meet both domestic and export needs. However, the export

of graphite from China primarily includes the primary product, while some part of more

processed graphite is imported from abroad. In addition, current recycling efforts are

primarily focused on cathode materials and the corresponding graphite recovery rate has been
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extremely low and led to resource loss.

Although the consumption of resources has almost doubled in 3 years, China continues to

depend on imports of Li, Co and Ni from aboard. The most critical materials in LIBs, Li and

Co, depend most heavily on importation. The biggest problems for Ni and natural graphite

have been increasing production demands and resource waste, respectively. On the one hand,

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China needs a large amount of imported resources to produce LIBs for export. For example,

19.3 wt.% of LIBs were produced to satisfy exportation demands, while an additional 19.7 wt.%

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and 6.3 wt.% of LIBs were exported as part of CEs and EVs products, respectively. On the

other hand, the amount of stocks in use has accumulated over the years. In 2016, net increases

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of stored products during the consumption phase were 6.56 kt, 24.71 kt, 11.54 kt, and 80.44 kt.

In addition to the increase in usage demand, lack of proper collection meant that EoL products

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remained in the hands of consumers for many years after devices were replaced. Without
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effective collection and recovery measures, materials will remain in the consumption process

for longer, which will in turn result in low resource utilization and increased environmental
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pollution. Although both the recovery and collection rates have increased compared with 2013,

they are not adequate for dealing with the predicted surge in scrap products. Currently, it is
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important to direct e-waste collectors and recyclers to dispose of obsolete LIBs with special
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concern for the 4 critical materials. An integrated recovery and recirculation system should be

established by 2020 to deal with increasing LIBs scrap.

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4. Conclusions

With the rapid development of modern industries, supply of some critical materials might be
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insufficient to satisfy an anticipated increase in demand. In this study, a CRM-MFA model

was used to evaluate the life cycle of critical materials for a selected megasector. Using this
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method, we have gained insight into the critical material mass flows in the Chinese LIB

industry and provided reference data for resource scarcity and environmental concerns.

1) Nine elements widely used in LIB production were evaluated using modified EI and SR

values. Four materials, i.e., Li, Co (with high criticality, normalized SR·EI≥12), Ni, and

graphite (with medium-high criticality, normalized SR·EI≥3), were identified as the most

critical material for LIB production. As the direct guidance and good supplements to

MFA, CRM evaluation results were used to guide and supplement the MFA and could
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lead to a better, scientifically based analysis of the LIB industry.

2) In the MFA of the four critical materials, five main processes of the LIB life cycle were

identified within the system boundaries. The static flow processes from ore to final

products indicated that the production of LIBs consumed 9.5 kt Li, 16.7 kt Ni, 38.4 kt Co,

and 122.6 kt graphite in 2016, which were 2.38, 2.17, 1.51, and 2.24 times that used in

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2013, respectively. Approximately 21.4-31.6 wt.% of LIBs (including individual batteries

and batteries assembled in products) were produced for exportation. However, more than

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80 wt.% of Li and Co resources relied on imports, and the external dependence changed

little from 2013 to 2016 due to mineral mining capacities in China.

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3) From the dynamic analysis of the consumption process, it was estimated that a large

number of secondary resources are maintained in storage, while production currently

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relies on primary resources. The storage of LIB cathode materials in the Chinese
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consumption process has increased from 300.62 kt to 366.79 kt from 2013 to 2016. Using

a Weibull distribution model, it was predicted that a scrap boom is coming that will
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provide 89.20-133.54 kt/a cathode scrap in 2020 and 275.01-391.83 kt/a cathode scrap in

2025. Under the premise of continuous consumption of mineral resources, secondary

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resources from waste material flows should be an important supplement for the Chinese
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LIB industry in the future.

Critical material flows in China are in an unstable situation at present. A large number of
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secondary resources are found in stocks maintained in the consumption process, and

production of cathode materials relies on imports to satisfy both global and domestic
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consumption. Further, recent improvements in efficiency for collection and recovery are far

from adequate for dealing with a surge of waste scraps. Efforts should be made to reduce the
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flow of valuable materials into the environment. It is expected that establishment of a CRM

oriented EoL LIB waste management system will decrease risks in the resource supply chain

and promote worldwide sustainable use of critical materials.

5. Opportunities and challenges

In this study, trends in critical materials use in the Chinese LIB industry have been identified

using a new CRM-MFA model. If CRMs are to be identified for China, a complete analysis

across all applications is needed for universal evaluation of the industry. A complete analysis
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will also provide useful guidance for the development of recycling systems and policies. The

use of this model will make it possible to establish a complete CRM evaluation system for

more materials in China. Achieving this goal will have a significant impact on the material

flow management of the Chinese national economy. The use of this model also provides a

meaningful opportunity to explore environmental issues beyond CRM flow management of

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LIBs. The combination of MFA and environmental impact assessment is of great benefit when

seeking to develop a low-carbon economy, circular economy, sustainable development, and

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Extended Producer Responsibility (EPR). However, challenges remain. Global LIB

production is growing rapidly, especially in China. Such a growth rate raises corresponding

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problems pertaining to raw material supply and resource circulation. To meet the resource

balance of supply and demand, secondary resources play an important complementary role in

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the supply chain. If there is strong growth in battery demand, the waste management process
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can only provide a fraction of the secondary critical material resources. This study predicts

estimated amount of LIB scrap in the next 8 years and provides some guidance for the
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closed-loop management of LIBs. However, achieving a closed-loop process in practice

remains a great challenge for the future.

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Acknowledgments

The authors acknowledge the financial support on this research from National Key Research
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and Development Program of China (2017YFB0403300/2017YFB043305), National Natural

Science Foundation of China under Grant No. 51425405 and L1624051 and 1000 Talents
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Program of China (Z.S.).

Nomenclature
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LIB Lithium-ion battery

SR Supply risk
EI Economic importance
CEs Consumer electronics
EVs Electric vehicles
GES Grid energy storage
e-waste Electronic waste
MFA Material flow analysis
CRMs Critical raw materials
EC European Commission
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USGS United States Geological Survey
LFP LiFePO4
LCO LiCoO2
NCM/NCA LiNixCoyMn1-x-yO2/ LiNixCoyAl1-x-yO2
LMO LiMn2O4
LTO Li4Ti5O12
M The raw material/metal used in LIBs

yM The share of M cost in LIB industry

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s
xM ,s The share of raw material demand in the sector s , ∑x M ,s =1

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As The value of the corresponding using megasector

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SI M , s The substitutability of M in sector s

SI M The substitutability of M in LIB industry

ρM
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The fraction of demand that is met by recovered materials
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The concentration of production and the governance status at
HHIWGI , M
the country level
VA Value added
M

WGI c The World Governance Indicators of country c

Sc The fraction of worldwide production in country c

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TR M The trade reliance ratio

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Do The domestic production amount of M

Im The import amount
Ex
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The export amount

t Time series, typically ∆t = 1 year in this study
S [T ] The in-use stock at a time T
S [0]
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The initial value of the first invested year

FI (t ) The material inflow

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FO ( t ) The material outflow

Pn The different LIB products

cn The material concentration in the products

The total number of the LIB types considered, which is 4 in this

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study

f (T ) Lifespan functions with time series input t

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FO [ t ] The annual output of EoL LIBs

The amount of LIBs flowing into the consumption process in

FI [ t - T ]
(t -T ) year

The probability densities of waste scraps arising in the year t

f (T )
with a battery lifetime of T
HEVs Hybrid electric vehicles

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PHEVs Plug-in hybrid vehicles
BEVs Battery electric vehicles
Supplementary material

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Table S1 Publications of MFA about LIBs considered and their respective contents
Table S2 Economic importance and supply risk calculation results of the raw material in LIBs

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Table S3 Economic importance calculations of the raw material in LIBs
Table S4 Import and export of the four critical material resources
Fig. S1. Calculation principles and detailed processes of the criticality evaluation model

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Fig. S2 The reserve, production situation (bar plots) and trade reliance ratio (scatter plots) of
the five main resources in China
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Fig. S3 Time to market for new materials in LIB industry
Fig. S4 Lifetime distribution functions of LIBs used in (a) Low (b) High lifetime scenarios
Fig. S5 The growth rate of different cathode scraps generation on baseline scenario
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Table S5 Typical constitutions and compositions of the widely used LIBs

Fig. S6 General flow sheet of spent LIBs treatment processes
Fig. S7 Material flow Sankey diagram of Chinese LIBs economy in: (a) 2013, (b) 2016
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Highlights

Material Flow Analysis on Critical Raw Materials of Lithium-Ion Batteries in

China

1. MFA for multiple elements in LIB industry is still scattered.

2. A CRMs evaluation system was proposed to optimize the further MFA.

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3. Sankey diagrams of Li, Co, Ni and C reveal their status in Chinese LIB industry.
4. The stock and obsolete amount from 2012 to 2025 were estimated and forecasted.

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