Yong Nam Jo

The High Performance of Crystal Water Containing Manganese Birnessite Cathodes for Magnesium Batteries.

Rechargeable magnesium batteries have lately received great attention for large-scale energy storage systems due to their high volumetric capacities, low materials cost, and safe characteristic. However, the bivalency of Mg(2+) ions has made it challenging to find cathode materials operating at high voltages with decent (de)intercalation kinetics. In an effort to overcome this challenge, we adopt an unconventional approach of engaging crystal water in the layered structure of Birnessite MnO2 because the crystal water can effectively screen electrostatic interactions between Mg(2+) ions and the host anions. The crucial role of the crystal water was revealed by directly visualizing its presence and dynamic rearrangement using scanning transmission electron microscopy (STEM). Moreover, the importance of lowering desolvation energy penalty at the cathode-electrolyte interface was elucidated by working with water containing nonaqueous electrolytes. In aqueous electrolytes, the decreased interfacial energy penalty by hydration of Mg(2+) allows Birnessite MnO2 to achieve a large reversible capacity (231.1 mAh g(-1)) at high operating voltage (2.8 V vs Mg/Mg(2+)) with excellent cycle life (62.5% retention after 10000 cycles), unveiling the importance of effective charge shielding in the host and facile Mg(2+) ions transfer through the cathodes interface.

Tin phosphide-based anodes for sodium-ion batteries: synthesis via solvothermal transformation of Sn metal and phase-dependent Na storage performance.

There is a great deal of current interest in the development of rechargeable sodium (Na)-ion batteries (SIBs) for low-cost, large-scale stationary energy storage systems. For the commercial success of this technology, significant progress should be made in developing robust anode (negative electrode) materials with high capacity and long cycle life. Sn-P compounds are considered promising anode materials that have considerable potential to meet the required performance of SIBs, and they have been typically prepared by high-energy mechanical milling. Here, we report Sn-P-based anodes synthesised through solvothermal transformation of Sn metal and their electrochemical Na storage properties. The temperature and time period used for solvothermal treatment play a crucial role in determining the phase, microstructure, and composition of the Sn-P compound and thus its electrochemical performance. The Sn-P compound prepared under an optimised solvothermal condition shows excellent electrochemical performance as an SIB anode, as evidenced by a high reversible capacity of ~560 mAh g−1 at a current density of 100 mA g−1 and cycling stability for 100 cycles. The solvothermal route provides an effective approach to synthesising Sn-P anodes with controlled phases and compositions, thus tailoring their Na storage behaviour.

Environment-Friendly Cathodes Using Biopolymer Chitosan with Enhanced Electrochemical Behavior for Use in Lithium Ion Batteries

The biopolymer chitosan has been investigated as a potential binder for the fabrication of LiFePO4 cathode electrodes in lithium ion batteries. Chitosan is compared to the conventional binder, polyvinylidene fluoride (PVDF). Dispersion of the active material, LiFePO4, and conductive agent, Super P carbon black, is tested using a viscosity analysis. The enhanced structural and morphological properties of chitosan are compared to the PVDF binder using X-ray diffraction analysis (XRD) and field emission scanning electron microscopy (FE-SEM). Using an electrochemical impedance spectroscopy (EIS) analysis, the LiFePO4 electrode with the chitosan binder is observed to have a high ionic conductivity and a smaller increase in charge transfer resistance based on time compared to the LiFePO4 electrode with the PVDF binder. The electrode with the chitosan binder also attains a higher discharge capacity of 159.4 mAh g(-1) with an excellent capacity retention ratio of 98.38% compared to the electrode with the PVDF binder, which had a discharge capacity of 127.9 mAh g(-1) and a capacity retention ratio of 85.13%. Further, the cycling behavior of the chitosan-based electrode is supported by scrutinizing its charge-discharge behavior at specified intervals and by a plot of dQ/dV.

Surface Modification of the LiFePO4 Cathode for the Aqueous Rechargeable Lithium Ion Battery

The LiFePO4 surface is coated with AlF3 via a simple chemical precipitation for aqueous rechargeable lithium ion batteries (ARLBs). During electrochemical cycling, the unfavorable side reactions between LiFePO4 and the aqueous electrolyte (1 M Li2SO4 in water) leave a highly resistant passivation film, which causes a deterioration in the electrochemical performance. The coated LiFePO4 by 1 wt % AlF3 has a high discharge capacity of 132 mAh g-1 and a highly improved cycle life, which shows 93% capacity retention even after 100 cycles, whereas the pristine LiFePO4 has a specific capacity of 123 mAh g-1 and a poor capacity retention of 82%. The surface analysis results, which include X-ray photoelectron spectroscopy and transmission electron microscopy results, show that the AlF3 coating material is highly effective for reducing the detrimental surface passivation by relieving the electrochemical side reactions of the fragile aqueous electrolyte. The AlF3 coating material has good compatibility with the LiFePO4 cathode material, which mitigates the surface diffusion obstacles, reduces the charge-transfer resistances and improves the electrochemical performance and surface stability of the LiFePO4 material in aqueous electrolyte solutions.

Co-intercalation of Mg2+ and Na+ in Na0.69Fe2(CN)6 as a High-Voltage Cathode for Magnesium Batteries

Thanks to the advantages of low cost and good safety, magnesium metal batteries get the limelight as substituent for lithium ion batteries. However, the energy density of state-of-the-art magnesium batteries is not high enough because of their low operating potential; thus, it is necessary to improve the energy density by developing new high-voltage cathode materials. In this study, nanosized Berlin green Fe2(CN)6 and Prussian blue Na(0.69)Fe2(CN)6 are compared as high-voltage cathode materials for magnesium batteries. Interestingly, while Mg(2+) ions cannot be intercalated in Fe2(CN)6, Na(0.69)Fe2(CN)6 shows reversible intercalation and deintercalation of Mg(2+) ions, although they have the same crystal structure except for the presence of Na(+) ions. This phenomenon is attributed to the fact that Mg(2+) ions are more stable in Na(+)-containing Na(0.69)Fe2(CN)6 than in Na(+)-free Fe2(CN)6, indicating Na(+) ions in Na(0.69)Fe2(CN)6 plays a crucial role in stabilizing Mg(2+) ions. Na(0.69)Fe2(CN)6 delivers reversible capacity of approximately 70 mA h g(-1) at 3.0 V vs Mg/Mg(2+) and shows stable cycle performance over 35 cycles. Therefore, Prussian blue analogues are promising structures for high-voltage cathode materials in Mg batteries. Furthermore, this co-intercalation effect suggests new avenues for the development of cathode materials in hybrid magnesium batteries that use both Mg(2+) and Na(+) ions as charge carriers.

Synthesis of Ordered Mesoporous Phenanthrenequinone-Carbon via π-π Interaction-Dependent Vapor Pressure for Rechargeable Batteries

The π-π interaction-dependent vapour pressure of phenanthrenequinone can be used to synthesize a phenanthrenequinone-confined ordered mesoporous carbon. Intimate contact between the insulating phenanthrenequinone and the conductive carbon framework improves the electrical conductivity. This enables a more complete redox reaction take place. The confinement of the phenanthrenequinone in the mesoporous carbon mitigates the diffusion of the dissolved phenanthrenequinone out of the mesoporous carbon, and improves cycling performance.

Eco-friendly nitrogen-containing carbon encapsulated LiMn2O4 cathodes to enhance the electrochemical properties in rechargeable Li-ion batteries.

This study describes the synthesis of nitrogen-containing carbon (N-C) and an approach to apply the N-C material as a surface encapsulant of LiMn2O4 (LMO) cathode material. The N heteroatoms in the N-C material improve the electrochemical performance of LMO. A low-cost wet coating method was used to prepare N-C@LMO particles. The N-C@LMO was characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), high-resolution Raman spectroscopy (HR-Raman), field emission scanning electron microscopy (FE-SEM), and field emission scanning transmission electron microscopy (FE-TEM) with elemental mapping. Furthermore, the prepared samples were electrochemically studied using the AC electrochemical impedance spectroscopy (EIS) and the electrochemical cycler. XPS suggested that the N-C coating greatly reduced the dissolution of Mn and EIS showed that the coating greatly suppressed the charge transfer resistance, even after long-term cycling. The control of Mn dissolution and inner resistance allowed faster Li-ion transport between the two electrodes resulting in improved discharge capacity and cycling stability.

A facile and highly efficient short-time homogenization hydrothermal approach for the smart production of high-quality α-Fe2O3 for rechargeable lithium batteries

In the present work, we have synthesized zero-dimensional (0D) and three-dimensional (3D) iron oxide (α-Fe2O3) sub-micron particles using a one-pot hydrothermal approach. Morphological studies reveal that the as-synthesized spherical α-Fe2O3 (SFO) material consists of nanospheres with void spaces. The prepared SFO delivers a high specific surface area of 100.80 m2 g−1 and significantly increases the contact area between the electrode and the electrolyte. The initial galvanostatic specific capacity of the SFO materials was 1306 mA h g−1 at a current density of 100 mA g−1, which is superior to that of bare cubic α-Fe2O3 (CFO). Moreover, the mesoporous SFO shows a good cycling stability with a capacity retention rate of 91.4% after 100 cycles. These attractive results suggest that the mesoporous SFO shows a good electrochemical performance as a negative electrode material for high-performance Li-ion batteries.

Effect of acid scavengers on electrochemical performance of lithium–sulfur batteries: Functional additives for utilization of LiPF6

We investigated a novel approach for utilizing LiPF6 as the lithium salt for Li–S batteries and verifying its chemical reactivity with the main solvent. It is found that the main obstacle for the adoption of LiPF6 is the undesired acid-catalyzed, cascade-type polymerization reaction between cyclic ether components in the solvent and LiPF6. Therefore, several kinds of acid scavengers are proposed to enhance the chemical stability between the main solvent and LiPF6. Simple storage tests indicate that polymerization occurred as acid residue is removed from the electrolyte. Consequently, the cell with a modified electrolyte shows excellent discharge capacity and moderate retention based on its improved chemical stability. These results indicate that assuring the chemical stability is the most important factor to utilizing LiPF6 as the main lithium salt for a Li–S cell. Additionally, it is believed that an understanding of the nature of chemical reactivity will be beneficial to constructing more efficient electrolyte systems owing to enhanced electrochemical performance of many kinds of energy storage systems including Li–S, Li–air, and metal–air batteries.

Si Nanocrystal-Embedded SiO x nanofoils: Two-Dimensional Nanotechnology-Enabled High Performance Li Storage Materials

Silicon (Si) based materials are highly desirable to replace currently used graphite anode for lithium ion batteries. Nevertheless, its usage is still a big challenge due to poor battery performance and scale-up issue. In addition, two-dimensional (2D) architectures, which remain unresolved so far, would give them more interesting and unexpected properties. Herein, we report a facile, cost-effective, and scalable approach to synthesize Si nanocrystals embedded 2D SiOx nanofoils for next-generation lithium ion batteries through a solution-evaporation-induced interfacial sol-gel reaction of hydrogen silsesquioxane (HSiO1.5, HSQ). The unique nature of the thus-prepared centimeter scale 2D nanofoil with a large surface area enables ultrafast Li+ insertion and extraction, with a reversible capacity of more than 650 mAh g−1, even at a high current density of 50 C (50 A g−1). Moreover, the 2D nanostructured Si/SiOx nanofoils show excellent cycling performance up to 200 cycles and maintain their initial dimensional stability. This superior performance stems from the peculiar nanoarchitecture of 2D Si/SiOx nanofoils, which provides short diffusion paths for lithium ions and abundant free space to effectively accommodate the huge volume changes of Si during cycling.