Unusual pseudocapacitive lithium-ion storage on defective Co3O4nanosheets.

Secondary lithium-ion batteries are restricted in large-scale applications including power grids and long driving electric vehicles owing to the low specific capacity of conventional intercalation anodes possessing sluggish Li-ion diffusion kinetics. Herein, we demonstrate an unusual pseudocapacitive lithium-ion storage on defective Co3O4nanosheet anodes for high-performance rechargeable batteries. Cobalt-oxide nanosheets presented here composed of various defects including vacancies, dislocations and grain boundaries. Unique 2D holey microstructure enabled efficient charge transport as well as provided room for volume expansions associated with lithiation-delithiation process. These defective anodes exhibited outstanding pseudocapacitance (up to 87%), reversible capacities (1490 mAh g-1@ 25 mA g-1), rate capability (592 mAh g-1@ 30 A g-1), stable cycling (85% after 500 cycles @ 1 A g-1) and columbic efficiency (∼100%). Exceptional Li-ion storage phenomena in defective Co3O4nanosheets is accredited to the pseudocapacitive nature of conversion reaction resulting from ultrafast Li-ion diffusion through various crystal defects. The demonstrated approach of defect-induced pseudocapacitance can also be protracted for various low-cost and/or eco-friendly transition metal-oxides for next-generation rechargeable batteries.

High-Performance Mg-Li Hybrid Batteries Based on Pseudocapacitive Anatase Ti1-x Cox O2-y Nanosheet Cathodes.

Despite the proposed safety, performance, and cost advantages, practical implementation of Mg-Li hybrid batteries is limited due to the unavailability of reliable cathodes compatible with the dual-ion system. Herein, a high-performance Mg-Li dual ion battery based upon cobalt-doped TiO2 cathode was developed. Extremely pseudocapacitance-type Ti1-x Cox O2-y nanosheets consist of an optimum 3.57 % Co-atoms. This defective cathode delivered exceptional pseudocapacitance (maximum of 93 %), specific capacities (386 mAh g-1 at 25 mA g-1 ), rate performance (191 mAh g-1 at 1 A g-1 ), cyclability (3000 cycles at 1 A g-1 ), and coulombic efficiency (≈100 %) and fast charging (≈11 min). This performance was superior to the TiO2 -based Mg-Li dual-ion battery cathodes reported earlier. Mechanistic studies revealed dual-ion intercalation pseudocapacitance with negligible structural changes. Excellent electrochemical performance of the cation-doped TiO2 cathode was credited to the rapid pseudocapacitance-type Mg/Li-ion diffusion through the disorder generated by lattice distortions and oxygen vacancies. Ultrathin nature, large surface area, 2D morphology, and mesoporosity also contributed as secondary factors facilitating superior electrode-electrolyte interfacial kinetics. The demonstrated method of pseudocapacitance-type Mg-Li dual-ion intercalation by introducing lattice distortions/oxygen vacancies through selective doping can be utilized for the development of several other potential electrodes for high-performance Mg-Li dual-ion batteries.

Realization of High Energy Density Sodium-Ion Hybrid Capacitors through Interface Engineering of Pseudocapacitive 3D-CoO-NrGO Hybrid Anodes.

Sodium-ion hybrid capacitors (SHCs) have attracted great attention owing to the improved power density and cycling stability in comparison with sodium-ion batteries. Nevertheless, the energy density (<100 Wh·kg-1) is usually limited by low specific capacity anodes (<150 mAh·g-1) and "kinetics mismatch" between the electrodes. Hence, we report a high energy density (153 Wh·kg-1) SHC based on a highly pseudocapacitive interface-engineered 3D-CoO-NrGO anode. This high-performance anode (445 mAh·g-1 @0.025 A·g-1, 135 mAh·g-1 @5.0 A·g-1) consists of CoO (∼6 nm) nanoparticles chemically bonded to the NrGO network through Co-O-C bonds. Exceptional pseudocapacitive charge storage (up to ∼81%) and capacity retention (∼80% after 5000 cycles) are also identified for this SHC. Excellent performance of the 3D-CoO-NrGO anode and SHC is owing to the synergistic effect of the CoO conversion reaction and pseudocapacitive sodium-ion storage induced by numerous Na2O/Co/NrGO nanointerfaces. Co-O-C bonds and the 3D microstructure facilitating efficient strain relaxation and charge-transfer correspondingly are also identified as vital factors accountable for the excellent electrochemical performance. The interface-engineering strategy demonstrated provides opportunities to design high-performance transition metal oxide-based anodes for advanced SHCs.