A critical review of the circular economy for lithium-ion batteries and photovoltaic modules – status, challenges, and opportunities

Figures & data

Garvin A. Heath

Dwarakanath Ravikumar

Figure 1. Electricity generation by technology in 2020, 2035, and 2050 as simulated in the Solar Futures Study (reproduced with permission (DOE 2021)). Ref. = reference scenario; Decarb = decarbonization of the electric sector scenario; Decarb + E = electric sector decarbonization plus electrification of other parts of the economy; Bio = biomass, Geo = geothermal, Hydro = hydropower (including pumped hydro-storage), CT = combustion turbine, CSP = concentrating solar power. See SI Section S2.1 for further explanation).

Figure 2. Time series illustrating historical and forecasted global prices (dotted line, left vertical axis) and cumulative demand (shaded area, right vertical axis) for LIBs in stationary and transportation (EV) markets from 2010 to 2035. (BloombergNEF 2021). According to BloombergNEF, in the past decade the unit price for LIBs has dropped to less than 12% of what it was in 2010 and is expected to further decrease to about 4% of the 2010 price by 2035. As the price continues to decrease, LIB demand is projected to increase 44,000-fold from 2010 to 2035.

Figure 3. Projected annual global material demand for PV manufacturing in 2030 and 2050 relative to 2018 global supply, data extracted from (Carrara et al. 2020). Results for the low and medium scenarios from the International Energy Agency and the high scenario from the Institute for Sustainable Futures of the University of Technology Sydney are shown, where medium is the baseline scenario (see SI Section S2.1 for more information). Note that Te, Si, and Glass use the y-axis on the left side, whereas all others refer to the y-axis scale on the right side. The levels of projected demand for c-Si module bulk materials, Si and Ag, are below 2018 global supply. The projected Cd demand for CdTe modules also remains under 2018 availability. In contrast, the projected demand for Te in 2030 is over 4 times, and in 2050 over 6 times the 2018 supply.

Figure 4. Comparison of projected global demand and current supply for cobalt by sector (duplicated with permission from Campagnol et al. 2018). Demand for cobalt from the battery industry is forecasted to dominate cobalt demand by 2025. Furthermore, demand from all sectors by 2025 is projected to be 201 kt, more than double the supply available in 2018 (~95 kt). Demand versus supply projections like this have motivated research into how to recover metals from end-of-life technologies to dampen demand for virgin materials. (p.a. = per annum).

Table 1. R strategy description with examples from a manufacturer’s and consumer’s (for R0–R2) perspective (adapted from Potting et al. 2017 and supplemented by Morseletto 2020; Reike, Vermeulen, and Witjes 2018)

Circular Economy	CE Strategy		Description
	Smarter product use and manufacture. Parts of these strategies contribute to Design for Circularity	(R0) Refuse	Manufacturer: Avoidance of toxic or critical materials, or the design of processes to eliminate material waste. Consumer: Avoidance or reduction of the consumption of a product. Example: Lead-free or fluorine-free PV modules.
		(R1) Rethink	Manufacturer: Design of a product to be more use-intensive or circula (e.g., designing to be easier to disassemble or designing one product for multiple functions). We also include product-service systems and other novel business models here. Consumer: Management of a product to be more use-intensive such as through sharing or using it for multiple purposes. Example: Design of LIB binders that are easier to dissolve.
		(R2) Reduce	Manufacturer: Decrease in consumption of virgin materials (dematerialization) and avoidance of waste in the manufacturing process. Consumer: Utilization of best practices for use to extend a product's useful lifetime. Example: Design of LIB cathodes to use less cobalt.
	Extend lifespan of product and its parts	(R3) Reuse	Manufacturer: Use of the product again by a second customer for the same functionality or purpose. Example: Use of an EV LIB in another EV.
		(R4) Repair	Manufacturer: Restoration of defective, broken, or malfunctioning components with the overall goal of extending the lifetime of the product. Example: Repairing a cracked PV backsheet.
		(R5) Refurbish	Manufacturer: Improvement of the working condition, quality, or functionality of a multi-component product, with the result of upgrading the product or bringing it back to its original state. Example: Restoring a used LIB to its original working condition, and reuse in its original application(Green Car Reports 2018, Spiers New Technologies 2021)
		(R6) Remanufacture	Manufacturer: Disassembly and processing of a product into components of which one or more are reused in a product with the same functionality. Quality standards evaluated through inspection, cleaning, and testing of components, and processing can bring the component(s) to the level of functionality needed. Example: Re-lithiating cathode materials for use in a new LIB (which is called direct recycling).
		(R7) Repurpose	Manufacturer: Use of the product or its components again by a second customer for a different functionality or purpose. Example: Using decommissioned EV LIBs for stationary applications.
	Useful application of materials	(R8) Recycle	Manufacturer: Recovery of product materials, whereby materials do not retain original structure. Recycled materials can be used in the same or different applications. This typically occurs at product end of life, but can also occur in the manufacturing process. Example: Extracting silver from end-of-life PV cells.
		(R9) Recover	Manufacturer: Recovery of energy from the end-of-life waste of a product (e.g., through incineration). Ex: Pyrolysising LIB binders and PV encapsulants.
Linear Economy

Table 2. Inclusion criteria for each screen of the systematic literature review

	LIBs	PV
Screen 1: Search	In English Published after 1990 Document type is either a journal article, book series, book chapter (>5 pages), or technical report*
Search 2: Title and Abstract**	Relevant to CE or a CE strategy of lithium-ion or EV batteries NOT a comment on a prior publication NOT a duplicate of another publication	Relevant to CE or a CE strategy of photovoltaics NOT a comment on a prior publication NOT a duplicate of another publication
Screen 3: Full text	Relevant to CE of LIBs (e.g., must include CE strategy, LIB) CE strategy must be applied to a process or product that is specific to the LIB industry Focuses on vehicle or stationary energy storage applications Includes NCA, NMC, LFP, or LMO cathode chemistries Does NOT solely consider non-LIB to LIB open-loop recycling	Relevant to CE of PV (e.g., must include CE strategy, PV) CE strategy must be applied to a process or product that is specific to the PV industry Focuses on PV at the residential, commercial, or utility scale Includes CdTe or c-Si PV Does NOT solely consider non-PV to PV open-loop recycling
Screen 4: Results/Analysis	NOT a duplicate of the same analysis***

*The OSTI search was limited to technical reports and not other types of publications.

**Technical reports do not always provide abstracts, so summaries were used instead.

***When a potential duplicate was identified, and the results reported were the same in each, we only retained the later published work. If the publications had different methods or results, then both were included.

Figure 5. Global market projections of LIBs in the transportation and stationary energy storage markets categorized by cathode chemistry (IEA 2021c; Wood Mackenzie 2021). The largest fraction of demand is for NMC, driven by the transportation market, with projected 2040 demand being more than double the second highest chemistry, LFP. Furthermore, the demand for LIBs by the transportation sector in 2040 dwarfs the demand for stationary LIBs. The category “other” includes LMO and other chemistries that are still in early research and development phases. Sources: IEA (2021), [The Role of Critical Minerals in Clean Energy Transitions], All rights reserved. Wood Mackenzie (2021), [Battery Raw Materials Service – 2021 update to 2040: Demand – H1 2021].

Figure 6. Projection of global PV capacity (GWp) and market share (%) for c-Si and thin-film technologies, data extracted from (SPV Market Research, 2021) (Mints 2018). CdTe makes up the largest segment of thin-film technologies, with the U.S. CdTe manufacturer First Solar alone manufacturing 6 GW, or 3% of the PV market in 2020 (Miller, Peters, and Zaveri 2020). Together, c-Si and CdTe represent almost 100% of the annual capacity additions today through 2025. (Note: Results from SPV’s “conservative” scenario are shown).

Figure 7. Process by which the systematic literature review was performed, following Preferred Reporting Items for Systematic Reviews and Meta-Analyses (PRISMA) guidelines. Specific steps used certain database and computer programs (see color-coded legend). The total number of publications obtained from the searches is represented by n = universe. The number of publications included in each screening process is represented by n_{in_x}, where x represents the screen iteration (see left side labels). The number of publications excluded by each step is represented by n_{ex_x}. The values of n_{in_x} for each screen per technology can be seen in Figure 8. The criteria for inclusion at each step can be found in Table 2

Figure 8. Number of publications of the universe and those that passed each screen for LIBs and PV. “Universe” refers to all publications identified based on the search terms used in SCOPUS and OSTI cumulatively from all search rounds, and equals 1,354 for LIBs and 1,757 for PV.

Table 3. Classifiers and sub-classifiers of LIB and PV publications

Classifier	Sub-classifiers		Remarks (when clarification deemed helpful)
Indicators	Sustainability	Economic	Quantifies the cost of implementing a CE strategy through assessing the economic impact on an entity or population
		Environmental
		Social
	Circular Economy	Economic	Quantifies effectiveness or degree of circularity through quantification of the cost of a product or service after a CE strategy has been applied.
		Mass
		Lifetime Extension	Quantifies the extension of the lifetime (in units of time) added to LIB/PV resulting from a CE strategy
		Effort	Quantifies the labor, in units of time, for a CE strategy
CE Strategies	Refuse (R0)		Refer to Table 1 for all “R” definitions
	Rethink (R1)
	Reduce (R2)
	Reuse (R3)
	Repair (R4)
	Refurbish (R5)
	Remanufacture (R6)
	Repurpose (R7)
	Recycle (R8)
	Recover (R9)
Life Cycle Phase	Design
	Raw Material Extraction
	Manufacture
	Use
	End-of-Life		Starts with decommissioning
Scope of CE Solution(s)	Nano		Level of chemistry or technology
	Micro		Level of PV/LIB enterprise
	Meso		Level of industrial park, collaboration between PV/LIB industries
	Macro		Level of city, state, country, or globe
Scale of Operations	Lab
	Pilot
	Commercial
Study Type	Technology Development
	Life cycle assessment (LCA)		Quantifies environmental impacts considering the whole life cycle of a product
	Techno-economic analysis (TEA)		Analyzes components of cost for a process or product
	Policy/Standards
	Social Behavior
	Performance		Quantifies the efficiency and related concepts of a LIB/PV system or component after a CE strategy has been applied
	Other Analysis		Other quantitative analysis such as human toxicity, material flow, or facility optimization
Publication Type	Original Research
	Review
Recycling Type	Open-Loop		Recycled PV or LIB materials used as input for the manufacturing of other products.*
	Closed-Loop		Recycled PV materials used as input for PV manufacturing, or recycled LIB materials used as input for LIB manufacturing.
LIB Cathode Chemistry	LFP		LiFePO4
	LMO		LiMn2O4
	NCA		LiNiCoAlO2
	NMC		Li(NixMnyCoz)O2 Potential combinations of xyz: 111, 532, 622, 811
LIB Cell Component	Cathode		Positive electrode
	Anode		Negative electrode
	Electrolyte		Conductive medium for the movement of ions between electrodes
	Other		Any other component of a cell, can include current collectors, separators, binders, or cell housing
	Whole unit
LIB Component	Cell		Unit consisting of cathode, anode, electrolyte, and other components detailed above
	Module		Collection of cells
	Pack		Collection of modules
	System		Combination of the pack and other balance of systems components such as battery management system, cooling system, etc.
LIB Application	Vehicle		Used in electric vehicles
	Stationary		Used for stationary energy storage
PV Technology	c-Si		Crystalline silicon
	CdTe		Cadmium telluride
Materials Recovered (PV only)	Glass		Recovered from both c-Si and CdTe
	Encapsulant		Recovered from both c-Si and CdTe
	Silicon/Si wafer		Recovered from c-Si
	Aluminum		Recovered from both c-Si and CdTe
	Cadmium		Recovered from the CdTe cell
	Tellurium		Recovered from the CdTe cell
	Copper		Recovered from both c-Si and CdTe
	Silver		Recovered from c-Si cell
	Lead		Recovered as “Solder Metals” from both c-Si and CdTe
	Tin		Recovered as “Solder Metals” from both c-Si and CdTe
	Backsheet		Recovered from c-Si
	Aluminum frame		Recovered from c-Si
	Junction box/wiring		Recovered from both c-Si and CdTe

*Note: Studies solely focused on non-PV/LIB recycled materials to be used in PV or LIB manufacturing were screened out of our review (Screen 3), as the recycling of non-PV/LIB materials are not part of PV/LIB CE.

Figure 9. A systems diagram representing the CE strategies for the manufacturing (M), installation and use (U), and the collection and recycling (EOL) phases of the life cycle of LIB systems, which are depicted as black circles. Physical material flows, shown on the right side of the black circles with black lines, are the CE pathways traditionally depicted in systems diagrams; we have added digital platforms and information system (Info Sys) pathways in blue which can enable or enhance the material ones. Because a transition to renewable energy is a goal of the CE, we mark the life cycle phases that could incorporate renewable energy with Orange circles. The stakeholders include various actors who participate in and contribute towards the CE of LIB. The decision enablers include the different policies that incentivize the CE, and analytical tools, which help quantify the economic and environmental impacts of the CE. Allied industries manufacture non-LIB products which can either utilize secondary materials recovered from a CE for LIBs or supply secondary materials to be utilized in the manufacture of LIBs. (EV: Electric Vehicle, S: Stationary, PSS: product-service system, SOH: State of Health).

Figure 10. A distillation of pre-processing and metallurgical operations of selected commercial LIB (left) and PV (right) recyclers. Pre-processing (in Orange) and metallurgical (in green) operations are listed in the center. These operations typically occur sequentially from top down, however some recyclers perform them in different orders or can skip certain operations based on their specific process and target materials. A circle within a cell in a row indicates the operation corresponding to the row is used by the LIB or PV recycler. A blank cell in a row indicates the operation is not used by that recycler. (Umi = Umicore (Samarukha 2020; Velázquez et al. 2019), Akk = Akuuser (Pudas, Erkkila, and Viljamaa 2011; Akuuser 2021; Harper et al. 2019; Samarukha 2020; Velázquez et al. 2019), Due = Duesenfeld (Duesenfeld 2021; Hanisch 2019; Harper et al. 2019; Samarukha 2020; Velázquez et al. 2019), Rec = Recupyl (Harper et al. 2019; Meshram, Pandey, and Mankhand 2014; Recupyl 2013; Samarukha 2020; Velázquez et al. 2019), Ret = Retriev (Harper et al. 2019; Novis Smith and Swoffer 2013; Retriev Technologies 2021; Samarukha 2020; Velázquez et al. 2019), Ont = OnTo Technologies (BEST Magazine 2020; Samarukha 2020; Sloop et al. 2020; Velázquez et al. 2019), Sum = Sumitomo-Sony (Cardarelli and Dube 2007; Samarukha 2020; Velázquez et al. 2019), Acc = Accurec (Gratz et al. 2014; Samarukha 2020; Velázquez et al. 2019), Lit = Lithorec (Samarukha 2020), Bat = Battery Resourcers (Gratz et al. 2014; Samarukha 2020; Velázquez et al. 2019), Fre = FRELP/Sasil (Latunussa et al. 2016), Veo = Veolia (Veolia 2021a), Fir = First Solar (Sinha, Cossette, and Ménard 2012), Sol = SolarRecyclingExperts (SolarRecyclingExperts 2021)).

Figure 11. Prevalence (counts) of LIB CE strategies reported in original research publications (columns in top panel) along with corresponding prevalence (percentage) by cathode chemistry in each CE strategy (pie charts in bottom panel). “Exclusive” indicates that the publication reports only one sub-classifier or can be classified as only one study type, “Multiple” indicates that the publication reports multiple sub-classifiers or can be classified as multiple study types. (n = 332; note that for the pie charts, a given publication may report multiple chemistries. The total number of publications of the pie charts for the different CE strategies from Refuse (R0) to Recover (R9) are 1, 10, 2, 16, 4, 7, 69, 66, 232, and 2).

Figure 12. Annual count of the different LIB CE strategies which were reported in original research publications from 2000 to 2021. (n = 332). Note that publications that analyze multiple CE strategies were counted under each. Year of publication reflects a journal’s planned official publication date, even if made available on-line earlier. Thus, there were some publications released in December 2021, with official publication dates in 2022.

Figure 13. Counts of LIB CE publications based on the classifiers listed in Table 3: of Indicators (A), Life Cycle Phase (B), Scope of CE Strategy (C), Scale of Operations (D) or based on the study type (where E includes all publications and F just reviews). (See Figure 11 for explanation of “Exclusive” and “Multiple”. Count of analyzed publications in panels A–D is 332 original research publications, panel E is 444 total publications, and panel F is 112 review publications, all of which passed the four screens. Since reviews were further classified in (F), they were considered their own study type in (E) and categorized exclusively as reviews). (Life. Ext. = lifetime extension; Raw Mat. Ext. = raw material extraction; Tech. Dev. = technology development; Perf. = performance; LCA = life cycle assessment; TEA = technoeconomic analysis).

Figure 14. Counts of LIB CE original research publications based on the Cathode Chemistry (A) and Application (B). Frame (B) displays both the publication counts (left column chart) and proportion of publications from each chemistry (right side pie charts). (See Figure 11 for explanation of “Exclusive” and “Multiple”; n = 332.).

Figure 15. Counts of original research publications which applied CE strategies for different LIB Cell Components (A) and LIB Components (B). Explanations of “Exclusive”, “Multiple”, and “Not reported” can be found in Figure 11. Both graphs represent 332 original research publications, all of which passed the 4 screens.

Figure 16. A systems diagram representing the CE strategies for the manufacture (M), install and use (U), and the collect and recycle (EOL) phases of the life cycle of PV. For an explanation of the different CE strategies, the stakeholders, information and material flows and the legend used please refer to .Figure 9

Figure 17. Prevalence (counts) of CE strategies reported in original research publications (columns) along with corresponding prevalence (percentage) for PV technology in each CE strategy (pies). (See Figure 11 for explanation of “Exclusive” and “Multiple”. (n = 160). Note that for the pie charts, a given publication may report multiple technologies).

Figure 18. Annual count of the different CE strategies for PV systems which were reported in original research publications from 2000 to 2021. (n = 160. Note that publications that analyze multiple CE strategies were counted under each. The counts account for c-Si and CdTe, as well as publications that did not report which technology they studied. Year of publication reflects a journal’s planned official publication date, even if made available on-line earlier).

Figure 19. Materials recovered from recycling (A) c-Si PV modules (n = 69 publications), and (C) CdTe modules (n = 30) based on counts of publications reporting original research; and annual count of original research publications by the materials recovered from recycling of (B) c-Si PV modules and (D) CdTe PV modules. Note that the encapsulant is typically EVA, and “Al/Cu” refers to aluminum and copper inside of the module. (11 c-Si and 23 CdTe publications which studied recycling did not report the recovery of any material and thus were excluded from the graphs. See Figure 11 for explanation of “Exclusive” and “Multiple”).

Figure 20. Counts of PV CE publications based on the classifiers listed in Table 3: of Indicators (A), Life Cycle Phase (B), Scope of CE Strategy (C), Scale of Operations (D) or Study Type (where E includes all publications and F just reviews). (See Figure 11 for explanation of “Exclusive” and “Multiple”, and Figure 12 for explanation of abbreviations and acronyms. Count of analyzed publications in panels A–D is 160 original research publications, panel E is 181 total publications, and panel F is 21 review publications, all of which passed the four screens. Since reviews were further classified in (F), they were considered their own study type in (E) and categorized exclusively as reviews. Some publications were not able to be classified when they did not report that aspect. For each panel, publications not reporting, and thus excluded from the count displayed, are: (A) = 71; (D) = 8); with all of the other panels = 0 publications not reporting. Note that since a given publication could have analyzed both PV technologies, that publication will count towards both in the pie charts of panel D).

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