Jinju Song

Lithium–sulfur (Li-S) batteries are attractive next-generation energy storage systems owing to their high theoretical energy density of 2600 Wh/kg and earth-abundant, eco-friendly sulfur. However, their practical application is hindered by the insulating nature of sulfur, large volume changes during cycling, and the polysulfide shuttle effect. Herein, we designed a dual-confinement cathode architecture combining mesoporous carbon with earth-abundant titanium dioxide (TiO₂). Sulfur composites with 70 wt% sulfur loading were prepared. Structural characterization via X-ray diffraction (XRD) and Brunauer–Emmett–Teller (BET) analysis showed a well-developed mesoporous network in KB but not in TiO₂. XRD confirmed that sulfur and anatase TiO₂ coexist in the composites, with weaker sulfur peaks in the mixed host. UV-vis absorption spectra showed that nano-TiO₂ removes more Li₂S₆ from solution than KB. Electrochemical evaluations revealed that the dual-confinement composite architecture balances the fast redox kinetics of carbon against the polysulfide affinity of TiO₂. Consequently, the composite achieved a high initial discharge capacity of 1300.89 mAh/g at 0.1 C and stable cycling over 100 cycles at 0.5 C. Furthermore, ex situ XRD analysis revealed nearly complete sulfur conversion while maintaining TiO₂ structural integrity. These results demonstrate an optimal balance between electronic conductivity and polysulfide mitigation via a sustainable material strategy.

Direct recycling offers a promising alternative for regenerating spent Li‐ion batteries (LIBs); however, achieving high‐purity cathode and ensuring cost‐effectiveness remains challenging. Herein, we present an innovative integrated process that simultaneously enables delamination and relithiation of spent cathodes, Li _x Ni _0.6 Co _0.2 Mn _0.2 O ₂ and Li _x FePO ₄ , under open‐air conditions with minimal energy. By oxidizing diethylene glycol, a green solvent, the transition‐metal oxidation state in the cathode is effectively reduced, thereby facilitating Li reinsertion into the structure. Consequently, the formation of glycol aldehyde induces 100% electrode delamination, enabling a one‐pot restoration pathway. The reaction mechanism is elucidated using Proton nuclear magnetic resonance ( ¹ H‐NMR), Soft X‐ray absorption spectroscopy (soft‐XAS), and X‐ray absorption near‐edge structure spectroscopy (XANES), and the regenerated cathodes consistently recover over 99% of their electrochemical performance for both 2 and 50 Ah cells. Furthermore, the regeneration solution is reusable, requiring only Li salt supplementation. This study presents a practical, low‐cost, and environmentally friendly approach for advancing the scalability and feasibility of direct LIB recycling technologies.

In this study, we present a modeling approach to estimate the combined effects of cyclable lithium loss and electrolyte depletion on the capacity and discharge power fades of lithium-ion batteries (LIBs). The LIB cell based on LiNi_0.6Co_0.2Mn_0.2O₂ (NCM622) was used to model the discharge behavior in the multiple degradation modes. The discharge voltages for nine different levels of cyclable lithium loss and electrolyte depletion were measured experimentally. When there was no cyclable lithium loss, the 50% of electrolyte depletion brought about 5% reduction in discharge capacity at 0.05 C discharge rate, while it resulted in 46% reduction when it was coupled with 30% of cyclable lithium loss. The 50% of electrolyte depletion with no cyclable lithium loss caused 1% reduction in discharge power during 0.5 C discharge at the state of charge (SOC) level of 0.8, while it resulted in 13% reduction when it was coupled with 30% of cyclable lithium loss. The modeling results obtained by using the one-dimensional finite element method were compared with the experimental data. The justification of the modeling methods is demonstrated by the high degree of concordance between the predicted and experimental values. Using the validated modeling methodology, the discharge capacity and usable discharge power can be estimated effectively under various combined degradation modes of cyclable lithium loss and electrolyte depletion in the LIB cell.

Microbial electrosynthesis (MES) is a promising technology platform for the production of chemicals and fuels from CO₂ and external conducting materials (i.e., electrodes). In this system, electroactive microorganisms, called electrotrophs, serve as biocatalysts for cathodic reaction. While several CO₂-fixing microorganisms can reduce CO₂ to a variety of organic compounds by utilizing electricity as reducing energy, direct extracellular electron uptake is indispensable to achieve highly energy-efficient reaction. In the work reported here, Rhodobacter sphaeroides, a CO₂-fixing chemoautotroph and a potential electroactive bacterium, was adopted to perform a cathodic CO₂ reduction reaction via MES. To promote direct electron uptake, the graphite felt cathode was modified with a combination of chitosan and carbodiimide compound. Robust biofilm formation promoted by amide functionality between R. sphaeroides and a graphite felt cathode showed significantly higher faradaic efficiency (98.0%) for coulomb to biomass and succinic acid production than those of the bare (34%) and chitosan-modified graphite cathode (77.8%), respectively. The results suggest that cathode modification using a chitosan/carbodiimide composite may facilitate electron utilization by improving direct contact between an electrode and R. sphaeroides.

This paper reports a modeling methodology to predict the effect of the loss of cyclable lithium of a lithium-ion battery (LIB) cell comprised of a LiNi_0.6Co_0.2Mn_0.2O₂ cathode, natural graphite anode, and an organic electrolyte on the discharge behavior. A one-dimensional model based on a finite element method is presented to calculate the discharge behaviors of an LIB cell during galvanostatic discharge for various levels of the loss of cyclable lithium. Modeling results for the variation of the cell voltage of the LIB cell are compared with experimental measurements during galvanostatic discharge at various discharge rates for three different levels of the loss of cyclable lithium to validate the model. The calculation results obtained from the model are in good agreement with the experimental measurements. On the basis of the validated modeling approach, the effects of the loss of cyclable lithium on the discharge capacity and available discharge power of the LIB cell are estimated. The modeling results exhibit strong dependencies of the discharge behavior of an LIB cell on the discharge C-rate and the loss of cyclable lithium.