bluuebunny/crossref_metadata_2025_split huggingface dataset:
Battery Deactivation for Safe and Efficient Recycling
Authors: Mikita Riho , Suzumura Akitoshi , Kondo Hiroki 
Published: August 2024

With the substantial increase in the demand for lithium-ion batteries (LIBs) for the adoption of electrification to reduce CO2 emission, safe and efficient recycling of spent LIBs is essential to utilize LIBs sustainably1. In hydrometallurgy-based or direct LIB recycling systems, which are expected to become mainstream in the future because of their low environmental impacts, deactivation is a crucial pretreatment step to safely handle LIBs during the processes2, 3. However, a common deactivation method, in which an external short circuit is induced using electronic loads or conductive liquid, cannot deactivate LIBs with disconnected electrical circuits or metallic Li plating on the negative electrode surface, despite their high safety risks.
We propose the advanced deactivation method, injecting a redox mediator (RM) solution inside the LIBs. The RM delivers electrons from the negative electrode to the positive electrode by cycling the reduction and oxidation on the negative and positive electrodes, respectively (redox shuttle reaction), resulting in discharging LIBs. In other words, the RM causes a short circuit inside the LIB. Therefore, it is possible to discharge a LIB that cannot be discharged externally, for example, a LIB with disconnected electrical circuits due to a safety device operation. Furthermore, the RM can strip Li metal plated on the negative electrode even though it is “dead lithium.” This unique characteristic contributes to the improvement in the safety and the Li collection rate in the recycling processes. Additionally, in this presentation, the deactivation mechanism of LIBs and its relationship with the electrochemical properties of the RMs will be discussed. The present findings will be beneficial and helpful for designing RMs for deactivation of more and more diversified spent LIBs.

References

J. Neumann, et al.: "Recycling of Lithium‐Ion Batteries—Current State of the Art, Circular Economy, and Next Generation Recycling" Adv. Energy Mater.
12, (2022).

A. Kwade, et al.: "Recycling of lithium-ion batteries" The LithoRec Way, Switzerland: Springler International Publishing AG (2018).

H. Rouhi, et al.: "Voltage behavior in lithium-ion batteries after electrochemical discharge and its implications on the safety of recycling processes" Journal of Energy Storage
35, (2021).
Room Temperature Efficient Regeneration of Spent LiFePO4 by Direct Chemical Lithiation
Authors: Ouaneche Tassadit , Stievano Lorenzo , Sougrati Moulay Tahar , Guery Claude , Monconduit Laure , Recham Nadir 
Published: August 2024

The exponential production of lithium-ion batteries for electric vehicles (EVs) and electronic applications leads to the creation of a huge stock of batteries at the end of life. Considering the current economic, geopolitical and environmental context, the recycling of these spent batteries is becoming an urgent need in order to mitigate environmental pollution and limit the waste of valuable and critical resources1.
In this work, we report a rewarding direct recycling process of spent LiFePO4 cathode material by direct chemical lithiation in solution2. After safe opening of the spent commercial battery, a structural, morphological, spectroscopic and electrochemical characterization of the spent LFP cathode was carried out to identify the reason(s) of battery failure. The results obtained by XRD (Fig 1a) and Mössbauer spectroscopy (Fig 1b) show that the loss of lithium in the cathode (up to 50%) consumed during formation and growth of the SEI during cycling, is the major reason of the end of life of these batteries, in total agreement with the literature3.
To address the lithium shortage problem, a recycling process via direct chemical lithiation in organic solution at room temperature of the LFP cathode has been implemented. Lithium iodide (LiI) dissolved in several solvents such as acetonitrile, cyclohexane, ethanol, DMSO, methanol and propan-1,2-diol was used as both the reductant and the lithiation agent. The best results were obtained with the cathode regenerated in ethanol, which is also the most captivating and environmentally friendly solvent. The different characterizations of this regenerated cathode allow evaluating the efficiency of the regeneration process. Mössbauer spectroscopy (Fig. 2a) confirms the total reduction of FeIIIPO4 to LiFeIIPO4, while electrochemical characterization (Fig. 2b) shows encouraging properties with a reversible capacity of ~168 mAh/g for the regenerated LFP.

References:

(1) Neumann, J. et al.Recycling of Lithium‐Ion Batteries—Current State of the Art, Circular Economy, and Next Generation Recycling. Adv. Energy Mater.
12, 2102917 (2022).

(2) Ouaneche, T. et al. Room temperature efficient regeneration of spent LiFePO4 by direct chemical lithiation. 579, J. Power Sources (2023) 233248.

(3) Zhou, S. et al. Direct recovery of scrapped LiFePO4 by a green and low-cost electrochemical re-lithiation method. Green Chem.
24, 6278–6286 (2022).

Figure 1: a) XRD pattern and b) Mössbauer spectrum of the recovered LixFePO4 powder.

Figure 2: a) Mössbauer spectrum and b) Charge-discharge galvanostatic curve at C/10 of the regenerated LFP cathode as positive electrode vs. Li+/Li0 and its derivative curve.

Figure 1
Compact Energy Storage Devices Developed from Waste-Derived Electrodes via Facile Recycling Technology
Authors: Das Himadri Tanaya 
Published: August 2024

Indeed, the development of sustainable and renewable energy technologies is a critical aspect of addressing the challenges posed by pollution and climate change. Electrochemical energy storage devices, such as batteries and supercapacitors, play a crucial role in this transition by enabling the efficient storage and utilization of energy. The mention of nanomaterials-based electrodes highlights a fascinating area of research and innovation. Nanomaterials offer unique properties and advantages due to their small size, high surface area, short-diffusion path, rapid kinetics, enhanced conductivity, making them highly desirable for energy storage applications.
Recycling waste to electrodes in compact energy storage device represents a particularly exciting frontier. Integrating energy storage into advance technology can enhance the portability and convenience of power sources, especially in the context of emerging technologies like wearable electronics and smart devices. However, challenges such as scalability, cost-effectiveness, and environmental impact must also be addressed to ensure the widespread adoption of these technologies. The emphasis on carbon-based nanomaterials, including graphene, carbon quantum dots, and activated carbon, as electrode materials is noteworthy. These materials show promise not only as negative electrodes but also as positive electrodes when combined with metal oxides, hydroxides, or sulphides, demonstrating their versatility in energy storage applications. Additionally, the innovative use of waste recycling, such as tires, shoots, and dry cells, for extracting carbon aligns with the broader goal of creating an eco-friendly environment. The focus on developing carbon-based electrodes from recycled waste for energy storage devices is commendable, as it not only addresses environmental concerns but also contributes to the creation of stable and efficient energy storage systems. In conclusion, this work on the generation of efficient carbon-based electrodes (graphene derived from different waste materials) for energy storage devices, showcases a multidisciplinary approach that considers both environmental sustainability and technological advancement. This research has the potential to contribute significantly to the ongoing efforts to create a more sustainable and efficient energy landscape.
Key words: Recycling, Electrochemical, Carbon, Metal oxides, Energy storage, Compact devices
The Circular Path Towards Decarbonising the Li-Ion Battery Value Chain
Authors: Kallitsis Evangelos , Offer Gregory James , Edge Jacqueline 
Published: August 2024

The rapid transition to clean energy and electric mobility has led to an unprecedented demand for Li-ion batteries (LIBs), necessitating a comprehensive decarbonisation of their entire value chain to meet climate goals [1]. This talk takes a holistic view at the LIB production and recycling system to explore cradle-to-cradle decarbonisation strategies. The Life Cycle Assessment (LCA) framework is used to quantify the comparative importance of developments in battery manufacturing, raw material sourcing and battery recycling in reducing greenhouse-gas emissions (GHG) arising from the globally-distributed LIB value chain.
On the upstream side, sourcing low-carbon materials is found to reduce the GHG footprint of LIB manufacturing by up to a factor of 4, depending on raw material type and source, and battery chemistry [2]. The geographical links between battery Gigafactory location and GHG emissions are also explored, revealing substantial differences between US states, Chinese provinces and European countries, traced to the carbon intensity of electricity generation [2]. On the downstream side, hydrometallurgical and pyrometallurgical treatment options for end-of-life LIBs are shown to achieve a GHG benefit of up to 40%, when recovered materials are circulated back to LIB production [3].
The battery production and recycling LCA models are integrated to present a comprehensive sensitivity analysis on the effectiveness of LIB recycling in reducing GHG emissions. This is shown to depend on battery chemistry, with lithium iron phosphate material recovery achieving lower benefits, but also on the geographical specificity of key operations, directly affecting the type of materials being displaced through secondary routes. The talk concludes with an outlook to 2035, presenting scenarios to reduce the GHG emissions of the battery value chain through technological developments, improvements in manufacturing and the establishment of circularity.
References
[1] Kallitsis, E., Lander, L., Edge, J., Bravo Diaz, L., Brown, A., Kelsall, G., Offer, G., Korre, A., 2022. Safe and sustainable lithium-ion batteries. Imperial College London-Energy Futures Lab.
[2] Kallitsis, E., Lindsay, J., Chordia, M., Wu, B., Offer, G., Edge, J. , 2023. Think global act local: the dependency of global lithium-ion battery emissions on production location and material sources. Preprint available at Research Square.
[3] Kallitsis, E., Korre, A. and Kelsall, G.H., 2022. Life cycle assessment of recycling options for automotive Li-ion battery packs. Journal of Cleaner Production, 371, p.133636.
Material Dynamics of Nickel (oxy)Hydroxide As an Alcohol Oxidation Electrocatalyst
Authors: Siboonruang Tana , Crago Colin Flynn , Aleman Ashton M. , Ríos Isabela , Schröder Johanna , Jaramillo Thomas F. , Tang Maureen H. , Burke Stevens Michaela 
Published: August 2024

Electrochemical alcohol oxidation is an attractive reaction for renewable-energy driven production of value-added chemicals, like precursors for acrylic (acrolein from glycerol) and nylon (adipic acid from cyclohexanol). Implementing selective, earth-abundant catalysts for alcohol oxidation can improve electrolyzer efficiency and economics. For example, replacing the energy intensive oxygen evolution reaction (OER) in CO2 electrolyzers with alcohol oxidation can decrease operating voltage by about 0.85 V and reduce electricity requirements up to 53% while also reducing carbon emissions from chemical production.1 Electrochemical alcohol oxidation catalyzed by as synthesized nickel oxyhydroxide (NiOOH) is hypothesized to proceed through two pathways, a chemical, redox pathway preferred by aldehydes (geminal diols in alkaline electrolyte), and a potential dependent pathway preferred by alcohols.2 Many studies have focused on understanding reaction mechanisms and device performance, however, transition metal alcohol oxidation catalysts, such as NiOOH, are known to undergo reduction/oxidation, phase changes, and even dissolution in the same potential window as alcohol oxidation.3 It is still unclear how these processes affect catalyst material stability and electrochemical performance.
In this work, we probe the performance stability and material stability of Ni(OH)2 for alcohol oxidation in alkaline media through electrochemical cycling and chronoamperometry. We use a rigorously Fe-free environment to mitigate performance impacts from Fe-contamination common in non-purified alkaline electrochemical studies.4 We show that the rate of change of alcohol oxidation current density (mA cm-2) depends on reaction pathway (redox vs. potential dependent), alcohol concentration, and side chain structure. Using EC-MS and NMR, we also probe changes in performance in yield and selectivity by quantifying oxidation products, including oxygen gas. These changes in performance are correlated to material changes through monitoring dissolution with on-line ICP-MS. Furthermore, to disentangle the role of potential and reactant (e.g. alcohol or water) on stability, we elucidate oxidation state and local structural changes using in situ X-ray Absorption Spectroscopy (XAS). Insights from this rigorous model system are directly translatable to the broader goal of developing efficient, long-lasting catalysts for industrial deployment of electrochemical organic reactions powered by clean energy.

References.

Verma, Sumit, Shawn Lu, and Paul JA Kenis. Nature Energy 4.6 (2019): 466-474.2.

Bender, Michael T., and Kyoung‐Shin Choi. ChemSusChem 15.13 (2022): e202200675.

Klaus, Shannon, et al. The Journal of Physical Chemistry C 119.13 (2015): 7243-7254

Wei, Lingze, et al. ACS Catalysis 13.7 (2023): 4272-4282.
Leveraging Flow-Assisted Electrochemistry Toward Decarbonization of Cement Manufacturing
Authors: Chaurasia Shabdiki B. , Luo Dayou , Aravamuthan Sundar Rajan , Wei Jianqiang , Agar Ertan 
Published: August 2024

In an effort to decarbonize the global economy by 50% in 2030 and achieve net-zero carbon emissions by 2050, there is a dire need to electrify industrial processes [1]. Approximately 8% of global carbon emissions comes from cement production [2]. Considering the rising demand for cement due to infrastructure expansion, it is critical to develop new concepts for the decarbonization of cement production. With this goal in mind, our work explores the effectiveness of flow-assisted cement electrolysis as a replacement to conventional fossil fuel based high-temperature kilns in cement manufacturing plants [3].
In this study, we employ a scalable 3-channel flow-reactor with acidic anolyte, basic catholyte, and a neutral chemical flush in between to generate calcium hydroxide, Ca(OH)2 [4, 5], which is the key ingredient in cement manufacturing. The central channel is separated from either half cells by a cation exchange and an anion exchange membrane. The electrochemical performance of the proposed cement electrolyzer under a variety of operating conditions is investigated by considering the key variables in reactor design, including flow rate, temperature, catalyst choice and feed concentrations, to shed light into the practical challenges of running a 3-channel flow reactor. Our preliminary study indicates that membranes are possibly responsible for a significant fraction of the limited yields of Ca(OH)2. Specifically, the anion exchange membranes tested are susceptible to degradation in alkaline conditions displaying poor ionic conductance, whereas the cation exchange membranes allow significant water crossover. The findings from this study pave the way in understanding key components for cement electrolysis and other electrochemical systems employing 3-channel flow reactors.

References

DeAngelo, J., et al., Energy systems in scenarios at net-zero CO2 emissions. Nature Communications, 2021. 12(1): p. 6096.

Ellis, L.D., et al., Toward electrochemical synthesis of cement—An electrolyzer-based process for decarbonating CaCO3 while producing useful gas streams. PNAS, 2019. 117(23): p.12584.

Rissman, J., et al., Technologies and policies to decarbonize global industry: Review and assessment of mitigation drivers through 2070. Applied Energy, 2020. 266: p. 114848.

Perego, A., et al., Electrochemical Flow Reactor for Cement Clinker Production. ECS Meeting Abstracts, 2021. MA2021-02(27): p. 840.

Olsson, J.A., S.A. Miller, and M.G. Alexander, Near-term pathways for decarbonizing global concrete production.Nature Communications, 2023. 14(1): p. 4574.
Rational Design of LixSiOy-Based Pre-SEI through Thermal-Evaporated Li-Metal Prelithiated SiOx Anode Enabling Extremely Stable and High-Rate Lithium Microbatteries
Authors: Chen Yi-Xiu , Huang Bing Han , Liu Chuan-Pu 
Published: August 2024

Recently, silicon oxides families (SiOx) have been commercialized as high capacity anode materials growing rapidly owing to their natural resource abundance and low-cost.(1) However, both the poor electron/ionic conductivity, and quite low initial coulombic efficiency (ICE) (normally < 60%) limits the further development into next generation SiOx anodes. (2) To address these two critical issues, various pre-lithiation strategies have emerged and systematically investigated with significant progress.(3, 4) Here, we provide a facile approach to prelithiate SiOx films by optimizing RF power and precisely controlling Li-metal deposition to overcome the current challenges of SiOx anodes. We found a strong correlation between the surface chemical state of SiOx and the pre-formation of LixSiOy SEI layers. The optimal prelithiation strategy achieves remarkable rate performance of 72.8% at 20C, and extremely excellent long-term cycling performance of 54.2% over 5000 cycles at 10C. This study significantly promotes SiOx-based anodes development, offering a promising strategy for extreme fast-charging and long-term stability not only overcoming the limitations in microbattery but scalable to practical electrodes.
Reference:

Q. Mai, Chem. Soc. Rev., 48, 285 (2019).

M. L. Jiao, Y. F. Wang, C. L. Ye, C. Y. Wang, W. K. Zhang and C. Liang, J. Alloy. Compd., 842, 21 (2020).

R. M. Zhan, X. C. Wang, Z. H. Chen, Z. W. Seh, L. Wang and Y. M. Sun, Adv. Energy Mater., 11, 20 (2021).

X. Q. Min, G. J. Xu, B. Xie, P. Guan, M. L. Sun and G. L. Cui, Energy Storage Mater., 47, 297 (2022).
(Battery Student Slam 8 Award Winner) Evaluating Electrodeposited Tin and Antimony-Based Anodes for Sodium-Ion Batteries
Authors: Gallawa Jessica Ruby , Ma Jeffrey , Prieto Amy L 
Published: August 2024

The widescale adaption of intermittent renewable energy sources, such as wind and solar, must be accompanied by a grid storage network to store energy when it is abundant and redistribute it as needed for on-demand use. Short-term storage in the form of rechargeable batteries is an attractive avenue for meeting these storage needs. The dominant technology in today’s market, the lithium-ion battery (LIB), is cost-prohibitive due to the need for rare-earth materials. Using the same working principle as LIBs, sodium-ion batteries (NIBs) utilize earth-abundant, low-cost sodium compounds instead of lithium compounds. Tin (Sn) and antimony (Sb) alone are promising anode materials for sodium-ion batteries with high theoretical capacities (847 and 660 mAh/g for Sn and Sb with Na, respectively) relative to current LIB anode chemistry (372 mAh/g) [1,2]. When combined, SnSb has shown to have increased stability relative to Sn or Sb alone [3]. Here, we synthesized Sn-Sb thin films with varied Sn and Sb atomic ratios by co-electrodeposition from a deep eutectic solvent by modifying solution stoichiometry and electrodeposition parameters. Using a combination of X-ray photoelectron spectroscopy (XPS), X-ray diffraction, and energy dispersive X-ray spectroscopy (EDS), phases and compositions of Sn-Sb synthesized by electrodeposition were identified. Once synthesized, we sought to determine the influence of morphology, surface chemistry, and composition on the capacity retention and rate capabilities of Sn and Sb-based anodes in NIBs. An optimized electrode composition was identified using a carbonate-based electrolyte, which resulted in stable capacity retention cycling at a rate of C/2 for 270 cycles.
[1] W. T. Jing, C. C. Yang, and Q. Jiang, Journal of Materials Chemistry A, 8, 2913–2933 (2020).
[2] S. Megahed and B. Scrosati, Journal of Power Sources, 51, 79–104 (1994).
[3] W. P. Kalisvaart, H. Xie, B. C. Olsen, E. J. Luber, and J. M. Buriak, ACS Applied Energy Materials, 2, 5133–5139 (2019).
Developing High-Purity Sodium Oxychloride Solid-State Electrolyte for Sodium-Ion Batteries
Authors: Ly Karen , Zheng Fan , Smirnova Alevtina 
Published: August 2024

Sodium-ion batteries have attracted significant attention as an alternative energy source to lithium-ion batteries. Solid-state sodium oxyhalides (Na3OX, X = Cl, Br, I) have the advantages of easy synthesis from cheap raw materials. In this study, sodium oxychloride (Na3OCl) antiperovskite was synthesized using a microwave furnace, the first instance in currently available literature. Using the microwave furnace also significantly decreased the reaction time when compared to other published procedures. The ionic conductivity of Na3OCl pellets was determined using electrochemical impedance spectroscopy (EIS). Na3OCl was hot pressed between sodiated hard carbon in a PEEK lined split cell with stainless steel current collectors. The symmetric cell was tested at room temperature with varying external pressures (1 MPa to 12 MPa). Symmetric cells were also tested at constant external pressure (6 MPa) from room temperature to 80˚C.
Arrhenius plots demonstrated linear behavior in the whole temperature range with a calculated activation energy of 0.98 eV. The melting and crystallization temperatures were determined using differential scanning calorimetry (DSC). The purity of as-synthesized Na3OCl was evaluated using x-ray diffraction (XRD). The results on chemical composition and crystal-to-glass phase transformations were produced from in-situ X-ray diffraction (XRD) spectroscopy in the temperature range from 25˚C up to the melting point of Na3OCl. Cross-sectional SEM images of the Na3OCl pellets showed regions that were dense, but also regions with many pores (≤ 5 μm). SEM also showed microcracks that ranged from 1-5 μm. Future work will investigate methods of minimizing pores and microcracks during the cell manufacturing process as these surface features can impede efficient ionic movement.