Worldwide trends in mobile electrification, largely driven by the popularity of electric vehicles (EVs) will skyrocket demands for lithium‐ion battery (LIB) production. As such, up to four million metric tons of LIB waste from EV battery packs could be generated from 2015 to 2040. LIB recycling directly addresses concerns over long‐term economic strains due to the uneven geographic distribution of resources (especially for Co and Li) and environmental issues associated with both landfilling and raw material extraction. However, LIB recycling infrastructure has not been widely adopted, and current facilities are mostly focused on Co recovery for economic gains. This incentive will decline due to shifting market trends from LiCoO2 toward cobalt‐deficient and mixed‐metal cathodes (eg, LiNi1/3Mn1/3Co1/3O2). Thus, this review covers recycling strategies to recover metals in mixed‐metal LIB cathodes and comingled scrap comprising different chemistries. As such, hydrometallurgical processes can meet this criterion, while also requiring a low environmental footprint and energy consumption compared to pyrometallurgy. Following pretreatment to separate the cathode from other battery components, the active material is dissolved entirely by reductive acid leaching. A complex leachate is generated, comprising cathode metals (Li+, Ni2+, Mn2+, and Co2+) and impurities (Fe3+, Al3+, and Cu2+) from the current collectors and battery casing, which can be separated and purified using a series of selective precipitation and/or solvent extraction steps. Alternatively, the cathode can be resynthesized directly from the leachate.

A novel sodium hybrid capacitor (NHC) is constructed with an intercalationtype sodium material [carbon coated-Na 3 V 2 (PO 4 ) 3 , C-NVP] and high surface area-activated carbon derived from an eco-friendly resource cinnamon sticks (CDCs) in an organic electrolyte. This novel NHC possesses a combination of high energy and high power density, along with remarkable electrochemical stability. In addition, the C-NVP/CDC system outperforms present, well-established lithium hybrid capacitor systems in all areas, and can thus be added to the list of candidates for future electric vehicles. A careful optimization of mass balance between electrode materials enables the C-NVP/CDC cell to exhibit extraordinary capacitance performance. This novel NHC produces an energy density of 118 Wh kg −1 at a specifi c power of 95 W kg −1 and retains an energy density of 60 Wh kg −1 with high specifi c power of 850 W kg −1 . Furthermore, a discharge capacitance of 53 F g −1 is obtained from the C-NVP/CDC cell at a 1 mA cm −2 current density, along with 95% capacitance retention, even after 10 000 cycles. The sluggish kinetics of the Na ion battery system is successfully overcome by developing a stable, high-performing NHC system.

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In this study, we report a novel route via microwave irradiation to synthesize a bio-inspired hierarchical graphene--nanotube--iron three-dimensional nanostructure as an anode material in lithium-ion batteries. The nanostructure comprises vertically aligned carbon nanotubes grown directly on graphene sheets along with shorter branches of carbon nanotubes stemming out from both the graphene sheets and the vertically aligned carbon nanotubes. This bio-inspired hierarchical structure provides a three-dimensional conductive network for efficient charge-transfer and prevents the agglomeration and restacking of the graphene sheets enabling Li-ions to have greater access to the electrode material. In addition, functional iron-oxide nanoparticles decorated within the three-dimensional hierarchical structure provides outstanding lithium storage characteristics, resulting in very high specific capacities. The anode material delivers a reversible capacity of ~1024 mA · h · g(-1) even after prolonged cycling along with a Coulombic efficiency in excess of 99%, which reflects the ability of the hierarchical network to prevent agglomeration of the iron-oxide nanoparticles.

Novel Li-ion hybrid supercapacitors were developed containing composite cathodes of a conducting polymereither polyaniline (PANI) or polypyrrole (PPy)with Li(Mn 1/3 Ni 1/3 Fe 1/3 )O 2 nanoparticles. Activated carbon (AC) anodes were used in the presence of an organic electrolyte. Using a PANI composite electrode resulted in a cell with outstanding supercapacitive behavior, even at high currents.It showed better cycleability than the cells using a PPy composite electrode or pristine material. The cell with a PANI composite electrode delivered high specific capacitances of 140, 93, and 56 F g À1 at current densities of 0.72, 1.45 and 2.15 A g À1 , respectively. The observed capacitances are the best yet reported for hybrid supercapacitors based on Li-intercalating materials in organic electrolytes. The hybrid supercapacitor containing PANI delivered maximum energy and power densities of 49 W h kg À1 and 3 kW kg À1 , respectively. These results demonstrate the potential of developing polymer-encapsulated, Liintercalating materials for high-performance, Li-ion, hybrid supercapacitors.

A novel two-step surface modification method that includes atomic layer deposition (ALD) of TiO followed by post-annealing treatment on spinel LiNi Mn O (LNMO) cathode material is developed to optimize the performance. The performance improvement can be attributed to the formation of a TiMn O (TMO)-like spinel phase resulting from the reaction of TiO with the surface LNMO. The Ti incorporation into the tetrahedral sites helps to combat the impedance growth that stems from continuous irreversible structural transition. The TMO-like spinel phase also alleviates the electrolyte decomposition during electrochemical cycling. 25 ALD cycles of TiO growth are found to be the optimized parameter toward capacity, Coulombic efficiency, stability, and rate capability enhancement. A detailed understanding of this surface modification mechanism has been demonstrated. This work provides a new insight into the atomic-scale surface structural modification using ALD and post-treatment, which is of great importance for the future design of cathode materials.

For the first time, atomic layer deposition (ALD) of Al2 O3 was adopted to enhance the cyclic stability of layered P2-type Na2/3 (Mn0.54 Ni0.13 Co0.13 )O2 (MNC) cathodes for use in sodium-ion batteries (SIBs). Discharge capacities of approximately 120, 123, 113, and 105 mA h g(-1) were obtained for the pristine electrode and electrodes coated with 2, 5, and 10 ALD cycles, respectively. All electrodes were cycled at the 1C discharge current rate for voltages between 2 and 4.5 V in 1 M NaClO4 electrolyte. Among the electrodes tested, the Al2 O3 coating from 2 ALD cycles (MNC-2) exhibited the best electrochemical stability and rate capability, whereas the electrode coated by 10 ALD cycles (MNC-10) displayed the highest columbic efficiency (CE), which exceeded 97 % after 100 cycles. The enhanced electrochemical stability observed for ALD-coated electrodes could be a result of the protection effects and high band-gap energy (Eg =9.00 eV) of the Al2 O3 coating layer. Additionally, the metal-oxide coating provides structural stability against mechanical stresses occurring during the cycling process. The capacity, cyclic stability, and rate performance achieved for the MNC electrode coated with 2 ALD cycles of Al2 O3 reveal the best results for SIBs. This study provides a promising route toward increasing the stability and CE of electrode materials for SIB application.