2015; Wang, Wang, and Yang 2020), Use an optimal mix of transportation modes where possible (Hendrickson et al. 2021) to between 2 and 3 mm (VDMA 2019), and aluminum use can be reduced through frameless modules (Norgren, Carpenter, and Heath 2020). 2022). 2015). = per annum). J. Taiwan Inst. 2008), and designing the PV module to be more easily recyclable (e.g., using non-adhesive release layers) (Doi et al. 2021). 2021c). 2020). In closed-loop recycling, materials recovered from LIBs at EOL are reused in the manufacture of a new LIB (Gaines 2018; Harper et al. Metallurgy Rev. The series of steps involved in repurposing include collection at specific locations; presorting based on chemistry, design, and damage; disassembly and testing for degradation (Liao et al. doi: 10.1007/s10967-014-3556-5, Nan, J., Han, D., and Zuo, X. Finally, the cathode material was collected and reused (Figure 2C). (2014). 2017; Jung et al. 2018). A few examples can illustrate this. = technology development; Perf. The criteria for inclusion at each step for both LIBs and PV is shown in Table 1. Electric cars and batteries: How will the world produce enough? Waste Manage. Three CE strategies closed-loop recycling, open-loop recycling, and remanufacturing bring materials from the EOL phase back into the manufacturing phase of the LIB. Researchers have developed many discharge methods, such as the use of electrical conductors (e.g., metal chips, graphite, powders) (Nembhard 2020; Sommerville et al. 2020; Velzquez et al. Number of publications of the universe and those that passed each screen for LIBs and PV. Purify/Extract Metal: In the purification (also called metal extraction) step, the metal is purified through either hydrometallurgical, pyrometallurgical or direct recycling, which have been explained in preceding sections. As a result, we combine the discussion of these facets for LIB and PV systems in sections titled Stakeholders in the CE for LIB and PV, Decision enablers for the CE for LIB and PV, Renewable energy use for PV and LIB CE and Impact on ecological services in the PV and LIB CE, which appear in the PV results section below. The state of health and state of charge of legacy and more recently installed LIB systems which could impact the choice of CE strategy. Recycled PV materials used as input for PV manufacturing, or recycled LIB materials used as input for LIB manufacturing. As stated in the LIB section, recycling is an important CE strategy and is a backstop to avoid landfilling after other strategies have been exhausted. As will be elaborated in this article, the CE literature has generally coalesced around the classification of 10 CE strategies, of which recycling is but one. We would also like to thank Al Hicks for graphics support and Connor O'Neill for editorial support as well as Jen Walker, Jason Youngstrom and Claire Bolyard from the National Renewable Energy Laboratory library for helping us obtain scientific literature supporting this review. Figure 4. Several aspects of CE are motivated by market economics and are thus longstanding business practices. It is also generally advised to use lower-numbered R strategies first and only after exhausting those to proceed to higher-numbered R strategies (Potting et al. The third was not only using supercritical CO2 as extraction agent, but also includes electrolyte extraction and heating treatment. (See SI Section S2.2 for schematics of the construction of a typical c-Si PV module and LIB and see the Methods section for a discussion of different PV module technologies). Figure 1. 3099067 For example, the literature focuses most heavily on the EOL phases given that is where recycling is typically implemented (Figure 13 (b)). ), the development of high recovery rate, low energy consumption and low environmental hazard recycling process has a good commercial prospect. Unlike mass-based indicators which incentivize the recovery of bulk materials that contribute a significant share of the mass of the PV module, economic indicators emphasize the recovery of trace materials which are economically valuable but make an insignificant contribution to the mass of the module (e.g., silver). These include: Anticipatory LCA (Wender et al. 2020; Oreski et al. This is because by extending LIB lifetimes, the embodied energy, carbon emissions, cost, labor, etc. (2014). (2012). Figure 2. Once the universe was established, we screened the publications. Resynthesizing of lithium cobalt oxide from spent lithium-ion batteries using an environmentally benign and economically viable recycling process. What is the definition of a circular economy? This critical review embarked to understand the status, challenges, and opportunities of a CE for LIB and PV. Potential changes in recycling processes that affect material constituents and components for stationary LIBs (e.g., balance of systems components) (Pellow et al. We can also observe from Figure 11 that there is no consistent pattern of prevalence for certain chemistries to be favored in research of certain CE strategies, despite more publications overall on NMC chemistry (Figure 14 (a)). 2020; Gao et al. No. 2022), Identifying environmental (Ravikumar et al. (See Figure 11 for explanation of Exclusive and Multiple. After heating treatment at 650C, the electrochemical performance was improved, showing almost the same discharge capacity and energy density as the new material. Similarly for PV, the terms reuse and recover are used instead of recycle to define the processing of silicon from kerf (silicon ingot cutting losses). Clean. Figure 20. The terms used in the search query represented CE, CE strategies (R0R9, except the OSTI search which excluded R8), and either LIBs or PV, as well as synonyms that are commonly found in the literature for each. What research and other programs can help make a CE for PV and LIB succeed? Inclusion criteria for each screen of the systematic literature review. 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. 2021c), Beyond a limited body of literature for specific countries (Randell Environmental Consulting 2016, Song, Hu, Liang, et al. 2021). Process. N2025018 and N2025009), the National Natural Science Foundation of China (No. Figure 18. In the smelting reduction zone, the material is smelted into alloys of Cu, Co, Ni, and Fe, along with Li, Al, Si, Ca, and some Fe slag. 304, 395400. Since the CE for LIB will require transport of LIBs to recycling or other facilities (e.g., plants for remanufacturing, repurposing, etc. 2018; Samarukha 2020). (2020) went so far as to title a section of their article Deemphasize research and development on recovery of intact silicon wafers. Tao et al. 2020). In remanufacturing, individual components of the collected, spent LIBs are recovered, checked for quality standards, and reused in the manufacture of a new LIB. Figure 6. Lithium-ion batteries (LIBs) are a leading technology for providing electricity storage and are available on the market today at both residential and utility scales (Fluence 2022; Tesla 2022). Power Sources 77, 183197. How will existing fire, electric, and interconnection codes impact the use of repaired modules in rooftop and grid-tied settings? Non-recycling CE pathways are generally preferred in the CE hierarchy because they usually retain a greater proportion of the value of the original products (Richa, Babbitt, and Gaustad 2017). In the past few years, with the development of energy storage industry, LIBs with higher energy density and higher power output have been widely used in EVs. Technology development, underemphasizing many other aspects of a technology such as environmental, social, and economic performance as well as policy, regulation, behavior, and other aspects. 2017) decreasing the material requirements of PV manufacturing (e.g., eliminating ethylene-vinyl acetate) (Saint-Sernin et al. Blockchain-based platforms can be leveraged to implement smart contracts and link the supply from decentralized producers with the demand of decentralized consumers of PV electricity (Petri et al. This indicates a narrow focus on certain sub-classifiers with a lack of simultaneous analysis on how the CE for one sub-classifier impacts other sub-classifiers. Decommissioning is followed by non-destructive assessment to evaluate the mechanical integrity and electrochemical safety of the battery (Rallo et al. (2019). The results in Figure 17 show that the emphasis on PV recycling is significantly greater than other CE strategies: Recycling publications are greater in number than all other CE strategies combined, and even more skewed than for LIBs (Figure 11). 2021). In the spent electrode materials, the average content of Li is about 5 wt%, which is much higher than the content in natural ores and has recycling value. Considering the blowout development of EVs, the disposal of the huge amount of spent lithium-ion batteries (LIBs) brought about by the exhaustion of the life cycle of LIBs will soon become a huge problem that plagues society. 2021). Direct physical recovery technology has the advantages of short recovery route, low energy consumption, environmental friendliness and high recovery rate. With regard to addressing community concerns, socio-technical research can be particularly helpful. 2021a). Yet they are, by and large, not economically sustainable in current form and are certainly not at the capacity nor properly sited to have the impact that is needed now and in the near future to support a CE. This work was supported by the Fundamental Research Funds for the Central Universities (No. Then, the small cells were treated with supercritical CO2, and the electrolytes were extracted and treated in this process. Publicly available data, albeit limited, indicate that the value obtained from recovered materials of PV modules does not exceed the cost of recycling (Deng et al. 2017; Rallo et al. Due to the short history of LIBs, a systematic recycling system has not yet been formed. The impact of economic factors (e.g., market pricing, value of secondary materials). A comprehensive study on electrochemical performance of Mn-surface-modified LiNi0.8Co0.15Al0.05O2 synthesized by an in situ oxidizing-coating method. (See Figure 11 for explanation of Exclusive and Multiple. 2020), Optimizing siting of EOL infrastructure through geospatial analysis tools: EOL PV waste is going to be increasingly sourced from geographically disperse installation locations. 2020 The Authors. (n=332). doi: 10.1016/j.jpowsour.2013.11.092, Huang, B., Pan, Z., Su, X., and An, L. (2018). 2020), with unknown variability in these costs by geography. The second objective is to further separate bulk (e.g., glass, encapsulant, Si wafer, backsheet) and specialty materials from the sandwich.
Despite authors using conflicting terms, we classified each publication according to the definitions in Table 1. Changes in economic viability due to potential improvements in recycling processes. When carbon-free generation sources are used to charge the batteries in electric vehicles (EV), a pathway emerges to decarbonize transportation, which is currently the largest GHG-emitting sector in the United States (EPA 2021). 2019), Akk= Akuuser (Pudas, Erkkila, and Viljamaa 2011; Akuuser 2021; Harper et al. Recover includes the recovery of energy from the combustion of materials, such as the electrolyte and the organic materials including the separator and the plastics (Chen et al. 2021). System tradeoffs in siting a solar photovoltaic material recovery infrastructure, A green and environment-friendly gel polymer electrolyte with higher performances based on the natural matrix of lignin, European Photovoltaic Solar Energy Conference and Exhibition, Breaking free from cobalt reliance in lithium-ion batteries, Recycling of photovoltaic panels by physical operations, A closed loop process for recycling spent lithium ion batteries, Nissan begins offering rebuilt leaf battery packs. Standing Committee of the National Peoples Congress, Possibilities of use of glass recyclate from photovoltaic panels for concrete masonry units, Characterizing electric vehicle battery end-of-life fates for agent-based model of battery repurposing and recycling systems, American Center for Life Cycle Assessment Conference, Virtual, Location of facilities and network design for reverse logistics of lithium-ion batteries in Sweden, Assessing variability in toxicity testing of PV modules, Thermal treatment of waste photovoltaic module for recovery and recycling: Experimental assessment of the presence of metals in the gas emissions and in the ashes, The social-economic-environmental impacts of recycling retired EV batteries under reward-penalty mechanism, Recovering large-scale battery aging dataset with machine learning, Major challenges and opportunities in silicon solar module recycling, Second life and recycling: Energy and environmental sustainability perspectives for high-performance lithium-ion batteries, Simulating process-product interdependencies in battery production systems, The importance of design in lithium ion battery recycling A critical review, To shred or not to shred: A comparative techno-economic assessment of lithium ion battery hydrometallurgical recycling retaining value and improving circularity in LIB supply chains, Behaviour change in post-consumer recycling: Applying agent-based modelling in social experiment, 31st European Photovoltaic Solar Energy Conference and Exhibition, Faults and infrared thermographic diagnosis in operating c-Si photovoltaic modules: A review of research and future challenges, Towards a circular supply chain for PV modules: Review of todays challenges in PV recycling, refurbishment and re-certification, End-of-life pathways for photovoltaic backsheets, The lack of social impact considerations in transitioning towards urban circular economies: A scoping review, A critical review of lithium-ion battery recycling processes from a circular economy perspective, Recycling photovoltaic panels, a technology unique in France, Veolia opens the first European plant entirely dedicated to recycling photovoltaic panels, Repair options for PV modules with cracked backsheets. In addition, the supply of kerf as feedstock in open-loop recycling to allied industries (e.g., hydrogen production (Kao, Kao, Huang, and Tuan 2016), lithium-ion batteries (Kim et al. In the case of no recovery of electrolyte, the spent LIBs were disassembled, crushed and cleaned in the sealed box. 2021) and identify strategies to effectively communicate the goals and benefits. A better understanding of customer preferences and market conditions will help develop more effective business models (Svatikova et al. We have completed what we believe to be the most comprehensive review to-date in this domain, identifying 3,111 potentially relevant archival journal articles, book chapters, and government reports, and then classifying and analyzing the 444 LIB and 181 PV CE publications that passed through four objective screening stages. SWAVE is applied to each company, producing a score out of 20, with a higher number indicating that more materials can be recycled. doi: 10.1021/es302420z, Etacheri, V., Marom, R., Elazari, R., Salitra, G., and Aurbach, D. (2011). After lowering the temperature and pressure, CO2 can be separated from the electrolyte and the electrolyte can be regenerated. Manufacturer: Use of the product again by a second customer for the same functionality or purpose. We followed standard systematic review protocols outlined by the Cochrane Handbook and reported these methods by following PRISMA guidelines; this ensures that the process by which we performed this review is as transparent and reproducible as possible (PRISMA 2021a; The Cochrane Collaboration 2022). However, pyrometallurgical recycling is energy-intensive and requires control equipment for environmentally hazardous air emissions. The benefits of non-recycling CE strategies are important to better understand, especially in light of their expected growth worldwide (Engel, Hertzke, and Siccardo 2019; WEF 2018) and because a CE pathway preceding recycling can alter attributes such as form factor, material quantity and quality that can affect recycling outcomes such as profitability. Transparently reports results of literature screening. In closed-loop recycling, the following materials can be recovered from EOL PV panels and either can be reused directly to manufacture new PV panels or reused after subsequent purification: cadmium (Berger et al. In order to better develop recycling technology of LIBs, it is best to do the following aspects: (1) Classify LIBs well according to the type of electrode; (2) Do a good job in battery design to make it meet the conditions of easy regeneration; (3) Cooperation on the recovery of spent LIBs and relevant legislative work around the world. The key processes in direct recycling are: obtaining the black mass, separating CAM from other materials (e.g., Polyvinylidene fluoride (PVDF), graphite) through thermal and floatation processes, overcoming the PVDF binder to delaminate the CAM from the cathode, and regeneration of the degraded CAM through relithiation (e.g., solid-state relithiation, hydrothermal relithiation) (Ji et al. doi: 10.1016/S0304-386X(02)00167-6, Lee, S. K., and Lee, S. H. J. N. (2000). Therefore, the technology of Co recovery should be transferred to the comprehensive utilization of spent Li. It is fair to say that CE is not yet mature in the PV and LIB industries. In refurbishing, the LIB is collected, restored to its original working condition, and then used in its original application (Green Car Reports 2018; Spiers New Technologies 2021). At the same time, with the policy orientation and the convenience and benefits brought by EVs, the global EV market is developing rapidly. Similarly, effort-based metrics are better suited to quantify the effectiveness of CE strategies which require human labor. Thus, it is necessary to evaluate CE strategies using a holistic systems perspective to assess achievement of ultimate objectives, identify trade-offs in advance to inform decision-making, and align key factors influencing adoption. A review on environmental, economic and hydrometallurgical processes of recycling spent lithium-ion batteries. 2021). CE strategies such as refurbish, repair, and remanufacture are often used synonymously, along with additional terms such as recondition or renovation (Ciobotaru, Benga, and Vireanu 2021; Liu and Gong 2014). All stages in the life cycle of LIB and PV are expected to have trade-offs between positive and negative impacts to ecological services. doi: 10.1016/j.wasman.2007.01.010, Mohagheghi, V., Mousavi, S. M., Vahdani, B., and Shahriari, M. (2017). Study and design CE-related aspects of LIB and PV markets. Purification/metal extraction: The separated materials from within the sandwich (e.g., Si wafer, silver, lead, tin, copper, cadmium, and tellurium) can be further purified through electrochemical (Huang et al. 2017 and supplemented by Morseletto 2020; Reike, Vermeulen, and Witjes 2018), Table 2. Prioritize technology development, deprioritizing many other aspects of a technology such as environmental, social, and economic performance as well as policy, regulation, behavior, and other considerations. Based on our assessment of the state of current literature and scientific understanding, we recommend research move beyond its prior emphasis on recycling technology development to more comprehensively investigate other CE strategies, more holistically consider economic, environmental and policy aspects of CE strategies, increase leveraging of digital information systems that can support acceleration towards a CE, and to continue to study CE-related aspects of LIB and PV markets. doi: 10.1016/S0304-386X(98)00046-2, Zhu, J. It also entails trade-offs examples of which were identified in this article and for which a holistic, systems-based analytical approach will be required to further elucidate. 2013; Karas et al. The lack of cost-revenue balance is further aggravated by the absence of robust analysis on how heterogeneity in the design of PV modules (e.g., double glass versus backsheet glass, fluorinated versus non-fluorinated back sheets) will impact the recyclability of modules and the economic sustainability of future recycling operations. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for U.S. Government purposes. 2015), Performance diagnostic technologies: In the use phase, digital and information technologies can enable more efficient repair and thereby increase the functional life of in-use PV systems. A time series of CE strategies shows that 2021 is the only year displaying substantial interest in non-recycling CE strategies (Figure 18), with the exception of recover which has been studied fairly consistently since 2015. 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). This means that in some cases, classifier pattern observations for PV are based on very small sample sizes, and should be understood as less definitive until more research confirms them. The recycling methods described in the literature use the following processes: Hydrometallurgical recycling uses low-temperature chemical processes such as leaching, precipitation, ion-exchange, solvent extraction, and electrolysis to separate, recover and purify the metals from the black mass (Brckner, Frank, and Elwert 2020; Harper et al. 2021; Ravikumar et al. By lowering the cost to access PV electricity, PSS can have positive environmental and social justice outcomes such as easier and cheaper access to renewable energy in communities with lower incomes and energy poverty (Drury et al. This method can be used not only to recycle electrode materials, but also to recycle Li and Fe, etc. 2017; Reike, Vermeulen, and Witjes 2018) include consumer-based definitions for these CE strategies, so we included those definitions here for completeness. Policies could approach standardized designs as a mandate, or could create incentives for manufacturers to collaborate and share data in protected ways, even with consumers (e.g., through blockchain) (Melin 2021). doi: 10.1016/j.jhazmat.2016.12.021, Choubey, P. K., Kim, M. S., Srivastava, R. R., Lee, J. C., and Lee, J. Y (2016). Second, cost remains the greatest challenge for increased recycling in countries that have not mandated recycling. In addition, Choubey et al. In addition, we identified two sets of publications that were not recognized as duplicates, representing an error rate of 0.2% (out of the total 929 publications passing Screen 2 when the duplication check was performed). 2019), or to improve electrolytes that can suppress dendritic growth (Ahmad et al. doi: 10.1016/j.chemosphere.2009.08.040, Li, L., Chen, R., Sun, F., Wu, F., and Liu, J. Even for recycling, we note that a combined set of indicators can more holistically assess the effectiveness of the circularity of recycling processes. These pathways are less mature than the material pathways and can include: Design for circularity (DfC): DfC is considered one approach to rethink (R1), by incorporating CE principles into the design of the product or the manufacturing process with the goal of increasing the circularity of the product. 145, 36473667. Of course, it is also theoretically possible to employ closed-loop recycling, but this has proven more challenging given high material purity requirements and other specifications that are hard to meet with EOL PV modules (Heath et al. Miner. Transport only the smaller mass of black mass to centralized recycling facilities (electrive.com 2020, Slattery, Slattery, Dunn, and Kendall 2021). 2016), copper (Huang et al. (2016) reported the leaching performance at a concentration of 0.7M H3PO4 and 4% hydrogen peroxide (V/V), achieving a recovery of over 99% of Li and Co at 40C for 1 h. The effect of ultrasonic and microwave on leaching reaction was studied (Shih et al., 2019). Another underrepresented strategy in the extant PV CE literature is the reduce strategy. Assessing the disparate siting and post-siting demographic change hypotheses of environmental injustice, Toward a cellchemistry specific life cycle assessment of lithiumion battery recycling processes, Estimation of recoverable resources used in lithium-ion batteries from portable electronic devices in Japan, Master of Science, KTH Royal Institute of Technology, A second life for electric vehicle batteries: Answering questions on battery degradation and value, A review on cellulose and lignin based binders and electrodes: Small steps towards a sustainable lithium ion battery, Design for recycling principles applicable to selected clean energy technologies- crystalline-silicon photovoltaic modules, electric vehicle batteries, and wind turbine blades. Power Sources. 2020) and TEA results (Deng et al. 2017, Ellen MacArthur Foundation 2022c). From a social impacts perspective, despite emerging studies (Markert, Celik, and Apul 2020), we find a lack of robust and comprehensive analysis on the social impacts of a CE for PV. 2020). ), regulatory clarity and consistency are required for LIB waste classification across different geographies through which the LIB is transported. Also, the first publications on repurpose appear in 2021. 2020). PV modules can be designed to include recyclable materials which enables more efficient recycling at end of life (DSM 2021). Eng. Organizations which specialize in recycling LIB and PV systems (Veolia 2021b; ROSI Solar 2022; We Recycle Solar 2022). 2019, Chen, Wang et al. Chemosphere 109, 9298. 2019). 2021b). In addition, the CE strategy of recover can be pursued in the EOL phase, wherein energy is recovered by the combustion of organic materials (e.g., ethylene-vinyl acetate and the backsheet) and used in the recycling process (Ardente, Latunussa, and Blengini 2019; Rubino et al. The total number of publications obtained from the searches is represented by n = universe. Sep. Purif. 20:312133. Considers not just material but also digital CE pathways. Yet, current literatures overwhelming emphasis on recycling is somewhat misdirected. Discharge: Removing electrical charge from each LIB is critical for worker and facility electrical safety. This lack of primary data inhibits study of the economic value of recovery of balance of systems materials, the assessment of feasibility of decommissioning and recycling the whole system, and any environmental trade-offs (Pellow et al. 2021), decreasing kerf losses though improved sawing methods (Kumar and Melkote 2018; Schwinde, Berg, and Kunert 2015), and kerf-free wafering (Henley et al. 2021), and thermal processes (Yu et al. Their review presents a list of principles, both general and specific for LIBs (and PV), which we have included in the SI Section S.4.3 because they are clear and succinct. Selective recovery of lithium from spent lithium iron phosphate batteries: a sustainable process. 2020). Here we highlight three opportunities to advance such research. For example, an EV LIB can be repurposed for use in a stationary energy storage application for such purposes as load levelling, transmission support, and grid frequency regulation (Ahmadi et al. The concentration on particular aspects of CE for LIBs is in some cases consistent with those topics market importance, and in other cases reveals which relevant aspects of CE for LIBs have been under-investigated, which raises opportunities for future research. Not yet. Separation in commercial LIB recycling facilities uses magnetism, density, size (screening), surface properties (e.g., froth floatation), and hydrolysis and filtration to concentrate the metals (Harper et al. Blockchain can also help manufacturers meet regulatory requirements (e.g., the European Union's requirement of recycling 70% of the mass of EOL LIBs by 2030) (Halleux 2021), for instance, by sharing LIB details with authorized recyclers, remanufacturers, and refurbishers. To better understand the status of the CE for PV and LIBs, data will need to be collected at regular intervals on both the markets for each of LIB and PV (e.g., changes to designs and materials inventory) and their developing CE markets. And other components can be extracted further. Digital platforms and information systems can be leveraged to implement and improve CE strategies across all three life cycle stages. 2022; Curtis et al. Although there are other important factors, especially socio-behavioral (Walzberg, Carpenter, and Heath 2021), as stated above, cost is a critical metric influencing adoption of CE strategies.
