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

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. This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.

AC C

EP

TE D

M AN U

SC

RI PT

ACCEPTED MANUSCRIPT

ACCEPTED MANUSCRIPT

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,* National Engineering Research Center of Distillation Technology, School of Chemical

RI PT

a

Engineering and Technology, Tianjin University, Tianjin 300072, China b

National Engineering Laboratory for Hydrometallurgical Cleaner Production

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

SC

China c

Macau Environmental Research Institute, Macau University of Science and Technology, Macau, SAR, 519020, China

National Development and Reform Commission, Beijing, 100824, China

M AN U

d

*Corresponding author: Zheng Lv ([email protected]); Zhi Sun ([email protected]) National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology Institute of Process Engineering, Chinese Academy of Sciences Tel: +86 10 82544844 Fax: +86 10 82544845

Abstract

TE D

No. 1 Beierjie, Zhongguancun, Haidian District, Beijing, China

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

EP

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

AC C

developed to identify the criticality associated with the supply risk (SR) and economic importance (EI) of different materials for the Chinese LIB industry. Dynamic materials flow 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

ACCEPTED MANUSCRIPT 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.

RI PT

Keywords: Lithium-ion batteries; dynamic material flow analysis; critical raw material; Weibull lifetime distribution; China

1. Introduction

SC

In recent years, the market for lithium-ion batteries (LIBs) has exhibited sustained and rapid growth. This growth can be attributed in part to the use of often updated consumer electronics

M AN U

(CEs), which require high-efficiency batteries (Hu et al., 2018; Zhang et al., 2017). Additionally, a large portion of the batteries used in electric vehicles (EVs) and used for grid 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 rechargeable battery market with an estimated 85% market share (excluding lead-acid

TE D

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

80

Energy storage in China Electric vehicles in China Consumer electronics in China Rest of the world, all applications

EP

Production amount of LIBs, GWh

et al., 2017) (Fig. 1).

70 60

AC C

50 40 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

ACCEPTED MANUSCRIPT 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

RI PT

countries due to its high flammability (Grant et al., 2013). LIB production continues to 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 worldwide suppliers, accounting for 50-70% of the total cost of LIBs (Gu et al., 2017). Across

SC

all applications, LIBs account for the greatest share of Li (75% in China and 46% worldwide, 2016) and Co consumption (76.6% in China and 44% worldwide) (CHYXX, 2016; USGS,

M AN U

2018). Mining efforts for these valuable resources has increased at a considerable rate, while the recovery volume of secondary resources does not occur at the same level. For example, 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, the international community should focus its concern on the supply safety and environmental

TE D

sustainability of LIB resources (Allwood et al., 2011; Helbig et al., 2018). Driven by the appeal of sustainable development and environmental protection, attention has been paid to the potential risks during the resource life cycle. To trace the material

EP

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

AC C

cycles in the anthroposphere. Using this method, the overall picture for essential resource or 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) 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

ACCEPTED MANUSCRIPT 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).

RI PT

When one material is used in many applications, the researchers have to dedicate a significant 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 calculated methods. Furthermore, few studies examined international trade flows across the

SC

whole life cycle of the various materials, failing to include materials that are imported or exported along with that of the electronic products. Such analyses may be difficult because

M AN U

data on different flows are not uniform, and data sources contain contradictory information. To fill these gaps and create a customized MFA for LIBs critical material flows on a country 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 LIB industry were identified. The analysis was constrained to China and focused only on the

TE D

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

EP

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

AC C

to boost the efficiency of resource use, and to support a future waste management system (Weil et al., 2018). 2. Methodology

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

ACCEPTED MANUSCRIPT 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.

RI PT

Since China has played a key role in both LIB production and recovery, this study defined the 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 the time period from 2010 to 2016 because the global EVs market experienced a significant

SC

surge during this time (Fig. 1). Since the advent of smartphones in 2011, the Chinese smartphone industry has entered a period of vigorous development; 2013 was used as the

M AN U

representative year for this new era of CEs. With the promulgation of the ‘Energy Saving and New Energy Vehicle Industry Development Plan (2012-2020)’ in China, the application of 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 reference period for the data used in the criticality assessments was based on the latest 4-year

TE D

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

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

EP

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

AC C

contains subcategories. For example, the raw materials preparation stage refers to physical 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 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.

ACCEPTED MANUSCRIPT International Market FI1

Mineral /Brine

F'M

FO1

Critical Raw Materials Preparation

FM

FL1

FI2

MxOy Mx(OH)y Mx(SO4)y Mx(CO3)y MxCly ……

F'P

FO2

LIBs Production

FP

FI3

FO3

LFP-C NCM-C LCO-C LMO-C F'E ……

Products Assembly

FL2

FE

FI4

CEs EVs GES

Consumption FU

In-use Stock

FL3

FL4

Waste Management (Recycle / Reuse) FL5 FR1

RI PT

FR2 FC

National Market

System Boundary

Transformation Flows

Loss Flows

Recovery Flows

SC

Material Trade Flows Products Trade Flows

2.2 Criticality evaluation factors

M AN U

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

CRMs are not only essential for the production of goods powered by LIBs in everyday use 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 one material influences the LIB industry and market. Generally, these factors include the

TE D

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

EP

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

AC C

and governance security. The model used to assess EI was derived in accordance to the model developed by the European Commission research group (EC, 2017). However, we focused 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:

ACCEPTED MANUSCRIPT EI M , LIB =y M

1 s ∑ ( xM ,s As SI M ,s ) GDP

(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

s

Note that

∑x

M ,s

RI PT

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

s.

= 1 was encompassed for all applications of the raw materials.

SC

The risks to M in the supply chain were caused by several factors: lack of substitutes, low recovery rates, high concentration and poor governance in primary production countries.

M AN U

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

SRM , LIB =SI M TRM (1 − ρM ) HHIWGI , M

(2)

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

TE D

of production and the governance status at the country level, i.e.:

HHIWGI ,M = ∑ ( Sc2WGI c )

(3)

c

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

EP

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

AC C

TRM indicates the trade reliance ratio: TRM =

D o+ Im − Ex Do

(4)

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

ACCEPTED MANUSCRIPT 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

RI PT

with contour lines (Glöser et al., 2015). The products of the two normalized indicators (SR·EI) 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 process that stores materials, so stocks in production or recycling factories could be neglected;

SC

the flow from raw materials to the final product was regarded as a continuous process. A static approach was applied to assess the material flows in the abovementioned stages (Fig. 3a).

M AN U

However, for the consumption process, products often stay in service for several years, and a few products would be considered stock after ending their life, so it is difficult to describe the 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 in-use stocks were regarded as a whole because they both stay in consumers’ hands before

AC C

EP

TE D

going onto subsequent stages.

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

ACCEPTED MANUSCRIPT 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)

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

S [T ] = S [0] + ∑ ( FI [t ] − FO [t ]) t =1

T

T

N

RI PT

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

t =1

t =1 n =1

SC

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

(6)

(7)

M AN U

where S [T ] is the in-use stock at a time T ; S[0] is the initial value of the first invested year; FI (t ) is the material inflow; FO (t ) is the material outflow; Pn presents the different LIB products; c n presents the material concentration in the products; N is the total number of the LIB types considered, which is 4 in this research.

TE D

For the material inflows, a rich set of historical data is accessible from the production process. However, there are different methodologies to quantify the outflows, including population 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

EP

be calculated based on the changes in the lifespan functions f (T ) with time series input t .

AC C

This approach is called population balance model or residence time model, which can be mathematically described as Eq. (8): Tmax

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.

ACCEPTED MANUSCRIPT (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

RI PT

To ensure the robustness and comparability of the results and maximize the quality of the 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 some import/export data or recycling information were not suitable for Chinese situation. So

SC

based on the CRMs data of EC (EC, 2017), the revised criticality methodology also combined with official Chinese data over that from trade/industry associations, other special interest

M AN U

groups and best estimation. Besides a detailed literature review, stakeholder consultations were also carried out, including the major LIB manufacturers, recycling companies, official management agencies in China.

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

TE D

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

EP

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

AC C

industry/market research in China after checking reasonable, some questionnaire survey, best 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 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)

ACCEPTED MANUSCRIPT USGS, National statistical data provided by the CNMIA (2014-2017)

Battery grade chemicals

Calculated according to the mass balance

CEs & EVs

Loss

Waste management

Selected material Waste in productive process Waste in consumption process Collection efficiency Recovery efficiency

3. Results and discussion 3.1 Criticality analysis

(Song, J. et al., 2017) (Zeng et al., 2015)

(Richa et al., 2017; Song, X. et al., 2017) (Li et al., 2017)

M AN U

In-use stock

Yearbook of Electric Power Industry in China (2014) Yearbook of the People's Republic of China (2014-2017) Calculated by upstream with Weibull lifetime distribution equation

RI PT

LIBs

SC

Domestic production

Mineral

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

TE D

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

AC C

EP

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

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.

ACCEPTED MANUSCRIPT 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
RI PT

yellow area of Fig. S1b). The dots with (SR·EI≤3) represent the non-critical raw materials (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 consideration of element location and matrix partitioning. Resilience scores of approximately

SC

20% below the medium-high SR·EI curve and above the high SR·EI curve were set to avoid problems with underestimating a material’s criticality. The final results of the CRM

M AN U

evaluation are shown in Fig. 4. CRMs for LIBs were classified and highlighted by blue dots in the criticality zone. Based on these results, we chose 4 materials (Li and Co with high 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 detail and discussed the bottleneck issues.

TE D

3.2 Process analysis of CRM-MFA

AC C

EP

3.2.1 Raw material mining and preparation

M AN U

SC

RI PT

ACCEPTED MANUSCRIPT

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

TE D

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

EP

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

AC C

supply chain of critical resources could breakdown suddenly due to economic or political 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 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.

ACCEPTED MANUSCRIPT 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

RI PT

Commercially, cathode materials vary significantly, while graphite is typically used as the 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 materials, i.e., LiCoO2 (LCO), LiMnO2 (LMO), LiNixMnyCo1-x-yO2 (NCM), LiNixCoyAl1-x-yO2

SC

(NCA). Fig. S3 shows major innovations in material technology for past, current and expected battery chemistries. From the earlier LMO, LCO, and LFP to the current NCM/NCA

M AN U

and even Li4Ti5O12 (LTO) batteries, LIB materials have been continuously updated to meet demands. The use of cheaper materials is the trend for the future. High-priced and scarce Co 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 main cathode materials in China from 2013-2016. Typical compositions of the four LIB types

TE D

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

EP

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

AC C

"high Ni and low Co". NCM333, NCM523, NCM622 and NCM811/NCA accounted for 13%, 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.

RI PT

ACCEPTED MANUSCRIPT

SC

Fig. 6. Production amount of 4 prototypical cathode materials in China from 2013 to 2016 3.2.3 Product assembly

M AN U

It is easy to determine material flows classified by chemical composition using existing data, but there are not yet systematic and through descriptions of flows for specific applications in 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 development of technology, a great variety of CEs were created: mobile phones, laptop

TE D

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

EP

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

AC C

Approximately 65.8 wt.% of LIBs in China were used in EVs applications; this proportion 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 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).

ACCEPTED MANUSCRIPT

Mobile phone

Mobile phone

3

0.02-0.04

Laptop Tablet Digital camera

5.5 5.1

0.18-0.47 0.03-0.1

6.5

0.06-0.16

BEV

8

180-400

PHEV

8

100-280

Electric bicycle

5

5.2-15.0

2100 million 170 million 80 million 15.3 million 421.8 thousand 93.9 thousand

Export amount of China, 2016

55,250 5,200

46.2 billion USD 23.6 billion USD

1,680

-

126 billion USD 182 billion USD 25.2 million units

63,000

122,330 17,840

15.2 thousand units

101,000

M AN U

10 million

Import amount of China,2016

It is also possible to identify split-flows for Li, Co, Ni and graphite when LIBs are assembled 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 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

TE D

EVs

equipment. Along with progress in research and development, high Co prices made some 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

EP

Digital camera

applications, LFP may continue to play a role because of cost considerations and the orderly recovery of spent LIBs from EVs.

AC C

Computer

Approximate total consumption of LIBs, 2016 (metric tons)

Production amount in China, 2016 (units)

RI PT

Sub-type application

Typical LIB mass range in different products (kg)

SC

Application

Anticipated LIBs lifespan in the application (years)

31.3 thousand units

ACCEPTED MANUSCRIPT LCO

LFP

NCM/NCA

LMO

Other

Percentage (kWh/kWh,%)

100

80

60

20

0

CEs 2013

CEs 2016

EVs 2013

EVs 2016

GES 2013

GES 2016

SC

Applications, Year

RI PT

40

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

3.2.4 Consumption and in-use stock

M AN U

from 2013 to 2016

After the three steps described above, materials eventually reach the consumer. As mentioned 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

TE D

the battery capacity of a new energy vehicle is less than 80%, it will be scrapped (Richa et al., 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, especially in CEs, are reserved somewhere by consumers at the end of their service life rather

EP

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

AC C

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

400

Low lifetime scenario Baseline scenario High lifetime scenario

350 300

Baseline scenario

250

LFP NCM/NCA LCO LMO

200 150 100

RI PT

Annual waste LIBs cathode material generation in China (thousand metric tons)

ACCEPTED MANUSCRIPT

50 0

2012 2014 2016 2018 2020 2022 2024

Year

SC

Fig. 8. Estimation and forecast of changes in lithium-ion battery waste flows from 2012 to the future. Note: the bar chart is based on the baseline scenario.

M AN U

The generation of LIB waste keeps increasing year by year, and this situation has been extremely serious since 2013 (Fig. 8). Based on the model predictions of production, the 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 scrap generated in 2020 and 2025, respectively. The growth rates of both LFP and NCM/NCA

TE D

are decreasing (Fig. S5), and the period of explosive growth is nearing completion. NCM/NCA was predicted to be the fastest growing waste stream of cathode materials after

AC C

EP

2018.

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

ACCEPTED MANUSCRIPT 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

RI PT

e-waste is becoming a problem that requires greater attention. 3.2.5 Waste management

There are three potential streams for the treatment of spent LIBs: product reuse, material recovery, and waste disposal. It was estimated that the collection rate of spent LIBs was at an

SC

extremely low level worldwide. The collection rate of spent LIBs was 45% in the EU but lower than 40% in China (Knights and Saloojee, 2015). Most parts of the spent LIBs were

M AN U

discard in the environment, with no chance to flow into the waste management process. To meet the growing resource demands, an integrated waste management system should be 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 reducing the environmental impact of spent batteries, many effective methods were applied to

TE D

cope with the spent LIBs. The processes of frequently-used treatment approach, namely pyrometallurgical, hydrometallurgical, pyrometallurgical + hydrometallurgical, and other methods (e.g., ultrasonic, mechanical) (Fig. S6a). The Chinese government has certified 109

EP

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

AC C

scale (e.g., GEM, Haopeng, Bangpu), industry infrastructure had progressed a lot from 2013-2016. Through the investigation of the known recovery enterprises, approximate treatment capacity and recovery rate are shown in Fig. S6b and S6c. Currently, 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

ACCEPTED MANUSCRIPT 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.

AC C

EP

TE D

M AN U

SC

RI PT

3.3 Evaluation of the life cycle of different critical materials

EP

TE D

M AN U

SC

RI PT

ACCEPTED MANUSCRIPT

AC C

Fig. 10. Sankey diagram of material flows in the Chinese lithium-ion battery economy in 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 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).

ACCEPTED MANUSCRIPT 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

RI PT

brine, imports and domestic production of raw minerals primarily depend on ore. Moreover, 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 and high cost. This situation is very unfavourable for balancing resource supply chains and

SC

achieving a closed-loop process.

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

M AN U

scarce, and 89.0 wt.% of Co comes from imports (Fig. 10b). Co is mainly used in production of LCO and NCM/NCA batteries. To save costs but provide similar performance, Co in LIBs 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.

Ni is primarily used in NCM/NCA (98.1 wt.%) batteries because LiNiO2 batteries have been

TE D

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

EP

materials.

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

AC C

in LCO, 18.1 wt.% in LMO, 21.9 wt.% in NCM/NCA, and 34.6 wt.% in LFP. Here, graphite 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 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

ACCEPTED MANUSCRIPT 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

RI PT

have been increasing production demands and resource waste, respectively. On the one hand, 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.% and 6.3 wt.% of LIBs were exported as part of CEs and EVs products, respectively. On the

SC

other hand, the amount of stocks in use has accumulated over the years. In 2016, net increases of stored products during the consumption phase were 6.56 kt, 24.71 kt, 11.54 kt, and 80.44 kt.

M AN U

In addition to the increase in usage demand, lack of proper collection meant that EoL products remained in the hands of consumers for many years after devices were replaced. Without 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 pollution. Although both the recovery and collection rates have increased compared with 2013,

TE D

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

4. Conclusions

EP

established by 2020 to deal with increasing LIBs scrap.

AC C

With the rapid development of modern industries, supply of some critical materials might be 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 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

ACCEPTED MANUSCRIPT 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,

RI PT

and 122.6 kt graphite in 2016, which were 2.38, 2.17, 1.51, and 2.24 times that used in 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 80 wt.% of Li and Co resources relied on imports, and the external dependence changed

SC

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

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

M AN U

number of secondary resources are maintained in storage, while production currently relies on primary resources. The storage of LIB cathode materials in the Chinese 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 provide 89.20-133.54 kt/a cathode scrap in 2020 and 275.01-391.83 kt/a cathode scrap in

TE D

2025. Under the premise of continuous consumption of mineral resources, secondary resources from waste material flows should be an important supplement for the Chinese LIB industry in the future.

EP

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

AC C

production of cathode materials relies on imports to satisfy both global and domestic 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 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

ACCEPTED MANUSCRIPT 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

RI PT

meaningful opportunity to explore environmental issues beyond CRM flow management of 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 Extended Producer Responsibility (EPR). However, challenges remain. Global LIB

SC

production is growing rapidly, especially in China. Such a growth rate raises corresponding problems pertaining to raw material supply and resource circulation. To meet the resource

M AN U

balance of supply and demand, secondary resources play an important complementary role in the supply chain. If there is strong growth in battery demand, the waste management process 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 closed-loop management of LIBs. However, achieving a closed-loop process in practice

Acknowledgments

TE D

remains a great challenge for the future.

EP

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

AC C

Science Foundation of China under Grant No. 51425405 and L1624051 and 1000 Talents Program of China (Z.S.). Nomenclature LIB SR EI CEs EVs GES e-waste MFA CRMs EC

Lithium-ion battery Supply risk Economic importance Consumer electronics Electric vehicles Grid energy storage Electronic waste Material flow analysis Critical raw materials European Commission

ACCEPTED MANUSCRIPT United States Geological Survey LiFePO4 LiCoO2 LiNixCoyMn1-x-yO2/ LiNixCoyAl1-x-yO2 LiMn2O4 Li4Ti5O12 The raw material/metal used in LIBs

yM

The share of M cost in LIB industry

xM ,s

The share of raw material demand in the sector s ,

As

The value of the corresponding using megasector

SI M , s

The substitutability of M in sector

SI M

The substitutability of M in LIB industry

ρM

The fraction of demand that is met by recovered materials

RI PT

USGS LFP LCO NCM/NCA LMO LTO M

s

M ,s

=1

SC

∑x

M AN U

s

WGI c

The concentration of production and the governance status at the country level Value added The World Governance Indicators of country c

Sc

The fraction of worldwide production in country c

HHIWGI , M

Do

Im Ex

t

AC C

S [T ] S [0]

The trade reliance ratio

The domestic production amount of M The import amount The export amount Time series, typically ∆t = 1 year in this study The in-use stock at a time T The initial value of the first invested year

EP

TR M

TE D

VA

FI (t )

The material inflow

FO ( t )

The material outflow

Pn

The different LIB products

cn

The material concentration in the products

N

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

f (T )

Lifespan functions with time series input t

ACCEPTED MANUSCRIPT FO [ t ]

The annual output of EoL LIBs The amount of LIBs flowing into the consumption process in

FI [ t - T ]

(t -T ) year

HEVs PHEVs BEVs

RI PT

The probability densities of waste scraps arising in the year t with a battery lifetime of T Hybrid electric vehicles Plug-in hybrid vehicles Battery electric vehicles

f (T )

Supplementary material

References

TE D

M AN U

SC

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 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 Fig. S2 The reserve, production situation (bar plots) and trade reliance ratio (scatter plots) of the five main resources in China 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 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

AC C

EP

Allwood, J.M., Ashby, M.F., Gutowski, T.G., Worrell, E., 2011. Material efficiency: A white paper. Resour. Conserv. Recycl. 55(3), 362-381. Cheah, L., Heywood, J., Kirchain, R., 2009. Aluminum Stock and Flows in U.S. Passenger Vehicles and Implications for Energy Use. J. Ind. Ecol. 13(5), 718-734. Chen, W., Graedel, T.E., 2012. Anthropogenic cycles of the elements: a critical review. Environ. Sci. Technol. 46(16), 8574-8586. CHYXX, 2016. The status of Chinese cobalt industry development and Industrial demand forecast in 2016. http://www.chyxx.com/industry/201611/470783.html. (Accessed 1st Nov 2017). CHYXX, 2017. Current situation and forecast of the Chinese lithium-ion battery industry. http://www.chyxx.com/industry/201712/598460.html. (Accessed 1st Jan 2018). Daigo, I., Igarashi, Y., Matsuno, Y., Adachi, Y., 2007. Accounting for steel stock in Japan. ISIJ Int. 47(7), 1065-1069. EC, 2017. Study on the review of the list of critical raw materials - Criticality Assessments. https://publications.europa.eu/en/publication-detail/-/publication/08fdab5f-9766-11e7-b92d-0 1aa75ed71a1. Glöser, S., Tercero Espinoza, L., Gandenberger, C., Faulstich, M., 2015. Raw material criticality in the context of classical risk assessment. Resour. Policy 44, 35-46.

ACCEPTED MANUSCRIPT

AC C

EP

TE D

M AN U

SC

RI PT

Grant, K., Goldizen, F.C., Sly, P.D., Brune, M.-N., Neira, M., van den Berg, M., Norman, R.E., 2013. Health consequences of exposure to e-waste: a systematic review. Lancet Glob. Health 1(6), e350-e361. Gruber, P.W., Medina, P.A., Keoleian, G.A., Kesler, S.E., Everson, M.P., Wallington, T.J., 2011. Global lithium availability a constraint for electric vehicles? J. Ind. Ecol. 15(5), 760-755. Gu, F., Guo, J., Yao, X., Summers, P.A., Widijatmoko, S.D., Hall, P., 2017. An investigation of the current status of recycling spent lithium-ion batteries from consumer electronics in China. J. Clean. Prod. 161, 765-780. Hao, H., Liu, Z.W., Zhao, F.Q., Geng, Y., Sarkis, J., 2017. Material flow analysis of lithium in China. Resour. Policy 51, 100-106. Hatayama, H., Yamada, H., Daigo, I., Matsuno, Y., 2007. Dynamic Substance Flow Analysis of Aluminum and Its Alloying Elements. Mater. Trans. 48(9), 2518–2524. Helbig, C., Bradshaw, A.M., Wietschel, L., Thorenz, A., Tuma, A., 2018. Supply risks associated with lithium-ion battery materials. J. Clean. Prod. 172, 274-286. Helbig, C., Wietschel, L., Thorenz, A., Tuma, A., 2016. How to evaluate raw material vulnerability - An overview. Resour. Policy 48, 13-24. Hu, X., Cao, D., Egardt, B., 2018. Condition Monitoring in Advanced Battery Management Systems: Moving Horizon Estimation Using a Reduced Electrochemical Model. IEEE/ASME Transactions on Mechatronics 23(1), 167-178. Huang, C., Vause, J., Ma, H., Li, Y., Yu, C., 2014. Substance flow analysis for nickel in mainland China in 2009. J. Clean. Prod. 84, 450-458. Ibrahim, F.B., Adie, D.B., Giwa, A.-R., Abdullahi, S.A., Okuofu, C.A., 2013. Material Flow Analysis of Electronic Wastes (e-Wastes) in Lagos, Nigeria. J. Environ. Prot. 04(09), 1011-1017. Kleijn, R., Huele, R., Voet, E.v.d., 2000. Dynamic substance flow analysis_ the delaying mechanism of stocks, with the case of PVC in Sweden. Ecol. Econ. 32(2), 241–254. Knights, B.D.H., Saloojee, F., 2015. Lithium Battery Recycling – keeping the future fully charged. Green Economy Research Report No. 1. Li, L., Fan, E., Guan, Y., Zhang, X., Xue, Q., Wei, L., Wu, F., Chen, R., 2017. Sustainable Recovery of Cathode Materials from Spent Lithium-Ion Batteries Using Lactic Acid Leaching System. ACS Sustain. Chem. Eng. 5(6), 5224-5233. Liang, Y., Su, J., Xi, B., Yu, Y., Ji, D., Sun, Y., Cui, C., Zhu, J., 2017. Life cycle assessment of lithium-ion batteries for greenhouse gas emissions. Resour. Conserv. Recycl. 117, 285-293. Liu, G., Muller, D.B., 2013. Mapping the Global Journey of Anthropogenic Aluminum: A Trade-Linked Multilevel Material Flow Analysis. Environ. Sci. Technol. 47(20), 11873-11881. Lu, B., Liu, J., Yang, J., 2017. Substance flow analysis of lithium for sustainable management in mainland China: 2007–2014. Resour. Conserv. Recycl. 119, 109-116. Muller, E., Hilty, L.M., Widmer, R., Schluep, M., Faulstich, M., 2014. Modeling Metal Stocks and Flows: A Review of Dynamic Material Flow Analysis Methods. Environ. Sci. Technol. 48(4), 2102-2113. Nitta, N., Wu, F., Lee, J.T., Yushin, G., 2015. Li-ion battery materials: present and future. Mater. Today 18(5), 252-264.

ACCEPTED MANUSCRIPT

AC C

EP

TE D

M AN U

SC

RI PT

Ongondo, F.O., Williams, I.D., Cherrett, T.J., 2011. How are WEEE doing? A global review of the management of electrical and electronic wastes. Waste Manage. 31(4), 714-730. Peterson, S.B., Apt, J., Whitacre, J.F., 2010. Lithium-ion battery cell degradation resulting from realistic vehicle and vehicle-to-grid utilization. J. Power Sources 195(8), 2385-2392. Pillot, C., 2015. The Rechargeable Battery Market and Main Trends 2014-2025, 32nd International Battery Seminar & Exhibit. Richa, K., Babbitt, C.W., Gaustad, G., 2017. Eco-Efficiency Analysis of a Lithium-Ion Battery Waste Hierarchy Inspired by Circular Economy. J. Ind. Ecol. 21(3), 715-730. Sommer, P., Rotter, V.S., Ueberschaar, M., 2015. Battery related cobalt and REE flows in WEEE treatment. Waste Manage. 45, 298-305. Song, J., Sun, Z., Gao, W., Wang, Y., Lin, X., Cao, H., 2017. Selective Recovery and Kinetics of Valuable Elements from Waste Lithium-ion Battery Cathodes (in Chinese). Chin. J. Process Eng. 17(4), 845-852. Song, T., Yang, Z., Chahine, T., 2016. Efficiency evaluation of material and energy flows, a case study of Chinese cities. J. Clean. Prod. 112, 3667-3675. Song, X., Hu, S., Chen, D., Zhu, B., 2017. Estimation of Waste Battery Generation and Analysis of the Waste Battery Recycling System in China. J. Ind. Ecol. 21(1), 57-69. State Council, PRC., 2017. Opinions on comprehensively strengthening ecological and environmental protection and resolute pollution prevention and control, in: 14th June 2018, p.13-14. Sun, X., Hao, H., Zhao, F., Liu, Z., 2017. Tracing global lithium flow: A trade-linked material flow analysis. Resour. Conserv. Recycl. 124, 50-61. Sun, Z., Cao, H., Xiao, Y., Sietsma, J., Jin, W., Agterhuis, H., Yang, Y., 2017. Toward Sustainability for Recovery of Critical Metals from Electronic Waste: The Hydrochemistry Processes. ACS Sustain. Chem. Eng. 5(1), 21-40. Swain, B., Kang, L., Mishra, C., Ahn, J., Hong, H.S., 2015. Materials flow analysis of neodymium, status of rare earth metal in the Republic of Korea. Waste Manage. 45, 351-360. USGS, 2017. Mineral Commodity Summaries of Lithium. https://minerals.usgs.gov/minerals/pubs/commodity/lithium/mcs-2017-lithi.pdf. USGS, 2018. Mineral Commodity Summaries of Lithium. https://minerals.usgs.gov/minerals/pubs/commodity/lithium/mcs-2018-lithi.pdf. Vaalma, C., Buchholz, D., Weil, M., Passerini, S., 2018. A cost and resource analysis of sodium-ion batteries. Nature Reviews 3, 18013. Wang, C., Chen, B., Yu, Y., Wang, Y., Zhang, W., 2017. Carbon footprint analysis of lithium ion secondary battery industry: two case studies from China. J. Clean. Prod. 163, 241-251. Weil, M., Ziemann, S., Peters, J., 2018. The issue of metal resources in li-ion batteries for electric vehicles, in: Pistoia, G., Liaw, B. (Eds.), Behaviour of Lithium-Ion Batteries in Electric Vehicles. Battery Health, Performance, Safety, and Cost. . Springer, pp. 59-74. Weil, M., Ziemann, S., Schebek, L., 2009. How to assess the availability of resources for new technologies? Case study: Lithium a strategic metal for emerging technologies. Revue de Métallurgie 106(12), 554-558. Winslow, K.M., Laux, S.J., Townsend, T.G., 2018. A review on the growing concern and potential management strategies of waste lithium-ion batteries. Resour. Conserv. Recycl. 129, 263-277.

ACCEPTED MANUSCRIPT

AC C

EP

TE D

M AN U

SC

RI PT

Yi, S., Lee, H., Lee, J., Kim, W., 2018. Upcycling strategies for waste electronic and electrical equipment based on material flow analysis. Environmental Engineering Research. Yokota, K., Matsuno, Y., Adachi, Y., 2003. Integration of Life Cycle Assessment and Population Balance Model for Assessing Environmental Impacts of Product Population in a Social Scale.pdf. Int. J. Life Cycle Assess. 8 (3), 129-136. Zeng, X., Li, J., 2015. On the sustainability of cobalt utilization in China. Resour. Conserv. Recycl. 104, 12-18. Zeng, X., Li, J., Liu, L., 2015. Solving spent lithium-ion battery problems in China: Opportunities and challenges. Renew. Sust. Energ. Rev. 52, 1759-1767. Zeng, X., Zheng, H., Gong, R., Eheliyagoda, D., Zeng, X., 2017. Uncovering the evolution of substance flow analysis of nickel in China. Resour. Conserv. Recycl. Zhang, C., Jiang, J., Gao, Y., Zhang, W., Liu, Q., Hu, X., 2017. Charging optimization in lithium-ion batteries based on temperature rise and charge time. Appl. Energ. 194, 569-577. Ziemann, S., Müller, D.B., Schebek, L., Weil, M., 2018. Modeling the potential impact of lithium recycling from EV batteries on lithium demand: A dynamic MFA approach. Resour. Conserv. Recycl. 133, 76-85.

ACCEPTED MANUSCRIPT

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

EP

TE D

M AN U

SC

RI PT

MFA for multiple elements in LIB industry is still scattered. A CRMs evaluation system was proposed to optimize the further MFA. Sankey diagrams of Li, Co, Ni and C reveal their status in Chinese LIB industry. The stock and obsolete amount from 2012 to 2025 were estimated and forecasted.

AC C

1. 2. 3. 4.