Figure - available from: Batteries & Supercaps
This content is subject to copyright. Terms and conditions apply.
Lithium‐ion battery and electrode scrap life cycle in the strategy of direct recycling.
Source publication
The growing demand and production of lithium‐ion batteries (LIBs) have led to a critical concern regarding their resources and end‐of‐life management. Consequently, LIB recycling has emerged as a prominent topic in academia and in industries, driven by new worldwide governmental regulations and the increasing gap between the supply and demand of cr...
Citations
... This intricate material is then targeted for recycling due to its economic value, primarily stemming from the presence of high-value metals, in addition to addressing environmental concerns and mitigating resource scarcity [1]. Nonetheless, a great challenge arises from the composite material layers within a battery's electrode [2]. ...
Keywords: Pressurized CO 2 technology Phase behavior CO 2-TEP-acetone ternary mixture CO 2-TEP binary mixture CO 2-acetone binary mixture Direct recycling of Li-ion batteries A B S T R A C T The ternary mixture of carbon dioxide (CO 2), triethyl phosphate (TEP), and acetone enabled an efficient delamination of Li-ion battery (LIB) positive electrode inciting an interest to study the ternary mixture behavior. Pressurized fluids, such as CO 2 , are known to be beneficial in various chemical processes. However, the behavior of CO 2 , when mixed with TEP and acetone is not well understood, particularly under pressure and temperature conditions. This study investigates the behavior of CO 2 or nitrogen (N 2) in mixtures with TEP and acetone at various compositions, using experimental investigations of the ternary system. Experimental data covers four temperatures at 35 • C, 70 • C, 100 • C and 120 • C at a constant pressure of 100 bar. The phase behaviors of the binary and ternary mixtures were observed using a transparent reactor, while the compositions were analyzed in situ with Raman spectroscopy. Under isobaric conditions, a single phase was observed with CO 2 at 35 • C, both in the binary systems with either TEP or acetone, as well as in the ternary mixture. In contrast, a biphasic system was observed at higher temperatures (70 • C, 100 • C, and 120 • C) in all mixtures containing CO 2. Specifically, the biphasic condition at 55 • C at 100 bar, of the mixtures were semi-quantitatively investigated using Raman spectroscopy to probe the compositions in the vapor and liquid phases. These observations elucidate the crucial role of CO 2 in the delamination of the positive electrode in LIB using the TEP-acetone-CO 2 system enabling high efficiency, low solvent consumption, and a faster processing time.
... 10 Direct recycling intends to favorize the reuse of the cathode active materials without having to destroy the cells or to come back to the starting chemicals but still is rather confined to laboratory scale at the moment. 11 Given the high energetic cost of pyrometallurgy, hydrometallurgy currently has the upper hand in the choice for a recycling method. 9 It can generate high yields for the recovery of critical elements like Ni, Mn and Co, 12 but involves the use of corrosive chemicals (e.g. ...
The recycling of LiNi0.6Mn0.2Co0.2O2 cathode active material (CAM) from Li-ion batteries cannot avoid the presence of impurities in the recycled Ni-, Co-, or Mn sulfates. The precise understanding of the impurities influence on the resynthesis is of uttermost importance. To tackle this goal, this study simulated the resynthesis process by adding on purpose and separately Al-, Fe-, and Li-sulfate in the regular CAM synthesis. Their effects on the morphology, elemental composition, crystal structure, and electrochemical performances of Ni0.6Mn0.2Co0.2Mx(OH)2 and LiNi0.6Mn0.2Co0.2MxO2 were systematically investigated for x = 0.0005, 0.005, and 0.05. The in-house reference material synthesized via a coprecipitation reaction allowed to produce a well-characterized basis. Above xAl = 0.0005, the hydroxide secondary particles lost their spherical form and above xFe = 0.005, the crystal structure was affected. Both effects led to cell capacity decay, contrary to the discrete influence of Li. The absence of any positive effects reported by similar studies, the complexity of the various influences of these foreign ions and the limitations of the coin cells tests were pointed out. These results are a solid groundwork for future academic and industrial studies in the field of circular economy, by determining a tolerance threshold for each impurity.
... However, with targeted efforts, these rates can be reduced to 5% to 10%. 5 ...
... Henceforth, treating electrode production scraps like spent batteries would therefore be a strategic error rather than developing a dedicated recycling route, which could be more adaptable and present benefits from an economical and environmental point of view. 4 Moving away from traditional destructive methods like established pyrometallurgy and hydrometallurgy, which have limitations such as a limited yield, high water and energy consumption, and an increased environmental impact, 3,5−9 the focus shifts toward developing direct recycling processes. It offers the highest material recovery rate 10 and effectively reduces time, cost, and environmental consequences. ...
... The particles were dispersed in water under stirring and ultrasonication, with obscuration maintained at 5−6% for all measurements. Implementing dynamic light scattering, the results obtained are in volume weighted mean D [4,3]. The morphology of the recovered NMC622 loose powders was compared by using Scanning Electron Microscopy (SEM). ...
... Scrap electrodes consist of battery materials that are not assembled into a functional battery. These materials are typically deemed unusable for various reasons, including trimming from production, out-of-specication materials, assembly errors, in-development materials, etc. 31 Currently, these scraps, also known as prompt scrap or pre-consumer scrap, dominate the market and are deemed to retain considerable value, and their direct reuse seems more viable than other types that come from end-of-life products. 32 A critical step in the direct battery recycling of scrap electrodes involves devising efficient methods for delaminating and recovering the active material without compromising its properties. ...
Among various recycling methods, direct recycling has emerged as a promising approach for recovering battery materials and directly reusing them to reduce carbon emissions and enhance the sustainability of the battery production process. Our study unveils, for the first time, different separation techniques for the delamination and the efficient direct recycling of high-voltage spinel LiNi0.5Mn1.5O4 (LNMO) cathode materials from scrap electrodes, evaluating chemical, mechanical, and thermal separation techniques. The impact of the separation technique on the active material and the influence of the particle morphology and binder type (aqueous and organic solvent) on the outcomes of these separation techniques is assessed in terms of recovery yield, purity, and electrochemical performance. The recovered materials' physicochemical properties show minimal alterations after the recycling process. The investigated separation techniques allow the complete delamination of the electrodes and the recovery of around 90% of the active material. The recovered LNMO is used without further treatment for preparing new electrodes, which achieve 95% of the cycling capacity of pristine LNMO after 100 charge/discharge cycles. These lab-scale findings are validated on pre-pilot-line and commercial production-line-processed electrode scraps.
This study reveals a mechanical upcycling approach combined with electrode engineering to transform carbon nanofiber and polylactic acid-based 3D printing waste into functional 3D components for sustainable zinc–iodine batteries.
With global lithium-ion battery (LIB) production on the rise, production scraps — constituting 5 to 30 wt.% of total manufacturing output — are expected to remain a major waste stream until at least 2030. These scraps present a significant recycling challenge, necessitating effective and sustainable solutions. In this study, we conduct a life cycle assessment (LCA) of an innovative CO2-assisted direct recycling process for LIB positive electrode production scraps. Using NMC622 (LiNi0.6Mn0.2Co0.2O2) positive electrodes material as a case study, this paper describes the environmental benefits and impacts of the recovery of this material with direct recycling compared to other conventional treatments (incineration, pyrometallurgy and hydrometallurgy). Lab-scale modelling identifies energy consumption and solvent usage as key environmental hotspots. A scale-up framework is applied to provide valuable insights and guide the sustainable development of this emerging technology. Eco-design strategies and benchmarking indicate that direct recycling has the potential to reduce environmental impacts; however, advancements in process energy efficiency and material recovery rates are necessary to ensure its competitiveness with existing recycling methods and its ability to meet industry-quality standards.
The large-scale utilization of power batteries in electrical vehicles (EVs) rapidly depletes metal mineral resources, leading to a significant shortage of valuable metals such as nickel, cobalt, and lithium. To address this scarcity and lower production costs, an urgent need is to develop effective separation strategies for extracting metals from spent batteries. This is crucial for sustainable economic development and environmental protection. Here, we present a method for separating Ni and Co from the positive electrodes of Ni-M(H) and Li-ion batteries through ammonia coordination and oxidization. In this process, the metals are leached from the positive electrodes and transformed into ammine complexes. The divalent cobalt complex is oxidized by hydrogen peroxide or air, forming the trivalent cobalt ammine complex, while the nickel complex crystallizes from concentrated aqueous ammonia and is thus isolated. The remaining trivalent cobalt ammine complex is crystallized from the solution by the addition of hydrochloric acid. We successfully recovered 81.1 % nickel and 55.5 % Co from the spent positive mixture of Ni-M(H) batteries, and 83 %∼90 % Ni and 64 ∼ 96 % Co from Ni from the simulated positive electrode mixing solutions with the Ni/Co ratio of 10:1 to 6:5. When the NH4Cl/Ni2+ ratio is 4.7, the separation efficiency of Ni increases to 94.7 %. We then re-synthesized nickel hydroxide (Ni(OH)2) with the nickel complex and supercapacitive cobalt oxide (Co3O4) products. The resulting Ni(OH)2 demonstrates superior capacity and cyclic charge/discharge performance compared to commercial spherical Ni(OH)2 with an initial capacity of 163.4 mAh⋅g−1, increasing to 252.8 mAh⋅g−1 by the 25th cycle, and reaching 271.9 mAh⋅g−1 by the 100th cycle under a specific current of 800 mA⋅g−1. Meanwhile, the Co3O4 exhibits a capacitance of 306.6F⋅g−1 after the 10th cycle, which maintains 247.8F⋅g−1 after 1000 cycles and 204.8F⋅g−1 after 3000 cycles under a specific current of 1.0 A⋅g−1. Moreover, a preliminary analysis of economic feasibility indicates that the separation and regeneration process of Ni and Co is low-cost and potentially environmentally friendly.
