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1. The critical effect of water content in the electrolyte on the reversible electrochemical performance of Zn–VPO ₄ F cells

   https://doi.org/10.1039/D0TA01622E  

   Yaghoobnejad Asl, Hooman; Sharma, Shyam; Manthiram, Arumugam (May 2020, Journal of Materials Chemistry A)

   null (Ed.)

   The electrochemistry of the Zn–VPO 4 F system has been studied for the first time in both wet non-aqueous and aqueous zinc-ion electrolytes. It is shown that H + ions present in the electrolyte insert into the cathode host in preference to sluggish Zn 2+ ion insertion. Furthermore, it is demonstrated that while H 2 O as a source of H + is essential for proper cell operation, an aqueous electrolyte is detrimental to cathode stability due to extensive dissolution. 

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2. Analysis of Direct Recycling Methods for Retired Lithium-ion Batteries from Electric Vehicles

   https://doi.org/10.1016/j.procir.2023.02.118  

   Wang, Yu; Zhai, Qiang; Yuan, Chris (January 2023, Procedia CIRP)

   The rapid expansion of electric vehicle (EV) fleet calls for large number of lithium-ion batteries to be recycled at their end-of-life. Various recycling methods have been developed or under development to recover the high-value materials from retired lithium-ion batteries. Amongst these methods, direct recycling techniques have been developed and reported to recycle battery materials for reuse in new battery manufacturing since the electrochemical properties of the recycled materials can be fully recovered to the same level of pristine materials. In literature, innovative sintering processes have been developed to recover the composition and crystal structure of spent cathode materials; hydrothermal regeneration processes have been reported to regenerate the spent cathode materials in the solvents at a moderate temperature, followed by the high-temperature short annealing process. The regenerated cathode materials show the same specific capacity and cycling performance as those of pristine materials. The electrochemical regeneration method is applied to fully recover the electrochemical performance of cathode material with stable crystal structure. While the direct recycling techniques are still under development, their future applications in industry are still not clear. This study aims to classify and summarize state-of-the-art of the direct recycling methods, and evaluate the regenerated cathode materials’ performance and the application potential to be used for manufacturing of new lithium-ion batteries in future. The results will help increase understanding of the direct recycling technologies and facilitate the associated R&D for future industrial scaling-up of direct recycling processes for retired lithium ion batteries from electric vehicles. 

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3. Size-Dependent Reaction Mechanism of λ -MnO ₂ Particles as Cathodes in Aqueous Zinc-Ion Batteries

   https://doi.org/10.34133/2022/9765710  

   Tang, Zhichu; Chen, Wenxiang; Lyu, Zhiheng; Chen, Qian (February 2022, Energy Material Advances)

   Manganese dioxide (MnO 2 ) with different crystal structures has been widely investigated as the cathode material for Zn-ion batteries, among which spinel λ -MnO 2 is yet rarely reported because Zn-ion intercalation in spinel lattice is speculated to be limited by the narrow three-dimensional tunnels. In this work, we demonstrate that Zn-ion insertion in spinel lattice can be enhanced by reducing particle size and elucidate an intriguing electrochemical reaction mechanism dependent on particle size. Specifically, λ -MnO 2 nanoparticles (NPs, ~80 nm) deliver a high capacity of 250 mAh/g at 20 mA/g due to large surface area and solid-solution type phase transition pathway. Meanwhile, severe water-induced Mn dissolution leads to the poor cycling stability of NPs. In contrast, micron-sized λ -MnO 2 particles (MPs, ~0.9  μ m) unexpectedly undergo an activation process with the capacity continuously increasing over the first 50 cycles, which can be attributed to the formation of amorphous MnO x nanosheets in the open interstitial space of the MP electrode. By adding MnSO 4 to the electrolyte, Mn dissolution can be suppressed, leading to significant improvement in the cycling performance of NPs, with a capacity of 115 mAh/g retained at 1 A/g for over 500 cycles. This work pinpoints the distinctive impacts of the particle size on the reaction mechanism and cathode performance in aqueous Zn-ion batteries. 

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4. Structural impact of Zn-insertion into monoclinic V ₂ (PO ₄ ) ₃ : implications for Zn-ion batteries

   https://doi.org/10.1039/C9TA00716D  

   Park, Min Je; Yaghoobnejad Asl, Hooman; Therese, Soosairaj; Manthiram, Arumugam (March 2019, Journal of Materials Chemistry A)

   The zinc-ion battery (ZIB) has been a system of particular interest in the research community as a possible alternative to lithium-ion batteries (LIB), and much work has been devoted to finding a suitable host material. In this article, monoclinic V 2 (PO 4 ) 3 is investigated as a host material for reversible insertion of Zn 2+ . Initial chemical assessment via a facile microwave-assisted chemical insertion method indicates the possibility of Zn 2+ insertion into the host. Electrochemical assessment, however, exhibits a significant capacity fade. In-depth analysis on the average and local structure of Li 3 V 2 (PO 4 ) 3 , the empty host V 2 (PO 4 ) 3 , and the Zn-inserted V 2 (PO 4 ) 3 reveals that heavy distortion is induced upon Zn 2+ insertion into the V 2 (PO 4 ) 3 framework, which is believed to be a result of a strong host–guest interaction jeopardizing the structural integrity. This is further supported by the dissolution of most of the material during the chemical oxidation of the Zn-inserted V 2 (PO 4 ) 3 . The underlying structural inadequacy poses difficulties for monoclinic V 2 (PO 4 ) 3 to be a viable reversible host for Zn-ion batteries. This work suggests that not only the electrostatic repulsions of multivalent ions in a structure during diffusion, but also the structural stability of the host upon insertion of multivalent ions, must be considered for a better design of suitable host materials for multivalent-ion batteries. 

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5. Perspective: Design of cathode materials for sustainable sodium-ion batteries

   https://doi.org/10.1557/s43581-022-00029-9  

   Sayahpour, Baharak; Hirsh, Hayley; Parab, Saurabh; Nguyen, Long Hoang Bao; Zhang, Minghao; Meng, Ying Shirley (May 2022, MRS Energy & Sustainability)

   Abstract Manufacturing sustainable sodium ion batteries with high energy density and cyclability requires a uniquely tailored technology and a close attention to the economical and environmental factors. In this work, we summarized the most important design metrics in sodium ion batteries with the emphasis on cathode materials and outlined a transparent data reporting approach based on common metrics for performance evaluation of future technologies. Sodium-ion batteries are considered as one of the most promising alternatives to lithium-based battery technologies. Despite the growing research in this field, the implementation of this technology has been practically hindered due to a lack of high energy density cathode materials with a long cycle-life. In this perspective, we first provide an overview of the milestones in the development of Na-ion battery (NIB) systems over time. Next, we discuss critical metrics in extraction of key elements used in NIB cathode materials which may impact the supply chain in near future. Finally, in the quest of most promising cathode materials for the next generation of NIBs, we overlay an extensive perspective on the main findings in design and test of more than 295 reports in the past 10 years, exhibiting that layered oxides, Prussian blue analogs (PBAs) and polyanions are leading candidates for cathode materials. An in-depth comparison of energy density and capacity retention of all the currently available cathode materials is also provided. In this perspective, we also highlight the importance of large data analysis for sustainable material design based on available datasets. The insights provided in this perspective, along with a more transparent data reporting approach and an implementation of common metrics for performance evaluation of NIBs can help accelerate future cathode materials design in the NIB field. Graphical abstract 

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