Sustainable regeneration of high-performance LiCoO2 from completely failed lithium-ion batteries.

Utilising the solid-state synthesis method is an easy and effective way to recycle spent lithium-ion batteries. However, verifying its direct repair effects on completely exhausting cathode materials is necessary. In this work, the optimal conditions for direct repair of completely failed cathode materials by solid-state synthesis are explored. The discharge capacity of spent LiCoO2 cathode material is recovered from 21.7 mAh g-1 to 138.9 mAh g-1 under the optimal regeneration conditions of 850 °C and n(Li)/n(Co) ratio of 1:1. The regenerated materials show excellent electrochemical performance, even greater than the commercial LiCoO2. In addition, based on the whole closed-loop recycling process, the economic and environmental effects of various recycling techniques and raw materials used in the battery production process are assessed, confirming the superior economic and environmental feasibility of direct regeneration method.

Layer-by-Layer Electrode Fabrication for Improved Performance of Porous Polyimide-Based Supercapacitors.

Nanoporous polymers are becoming increasingly interesting materials for electrochemical applications, as their large surface areas with redox-active sites allow efficient adsorption and diffusion of ions. However, their limited electrical conductivity remains a major obstacle in practical applications. The conventional approach that alleviates this problem is the hybridisation of the polymer with carbon-based additives, but this directly prevents the utilisation of the maximum capacity of the polymers. Here, we report a layer-by-layer fabrication technique where we separated the active (porous polymer, top) layer and the conductive (carbon, bottom) layer and used these "layered" electrodes in a supercapacitor (SC). Through this approach, direct contact with the electrolyte and polymer material is greatly enhanced. With extensive electrochemical characterisation techniques, we show that the layered electrodes allowed a significant contribution of fast faradic surface reactions to the overall capacitance. The electrochemical performance of the layered-electrode SC outperformed other reported porous polymer-based devices with a specific gravimetric capacitance of 388 F·g-1 and an outstanding energy density of 65 Wh·kg-1 at a current density of 0.4 A·g-1. The device also showed outstanding cyclability with 90% of capacitance retention after 5000 cycles at 1.6 A·g-1, comparable to the reported porous polymer-based SCs. Thus, the introduction of a layered electrode structure would pave the way for more effective utilisation of porous organic polymers in future energy storage/harvesting and sensing devices by exploiting their nanoporous architecture and limiting the negative effects of the carbon/binder matrix.

Flexible free-standing Ni-Mn oxide antenna decorated CNT/nanofiber membrane for high-volumetric capacitance supercapacitors.

There is growing demand for lightweight flexible supercapacitors with high electrochemical performance for wearable and portable electronics. Here, we spun nanoparticles of nickel-manganese oxides along with carbon nanotubes into carbon nanofibers and engineered a 3D networked Ni-Mn oxides/CNT@CNF free-standing membrane for flexible supercapacitor applications. The electrospinning process controlled the nanoparticle aggregation while subsequent heat treatment generates nanochannels in the fibres, resulting in a very porous tubular nanocomposite structure. The preparation process also enabled good interfacial contact between the nanoparticles and the conductive carbon network. The resulting Ni-Mn oxides/CNT@CNF membrane displays high mass loading (Ni-Mn oxides) of 855 mg cm-3 and low CNT incorporation of ∼0.4%. The outstanding porous structure, synergy of the carbon with Ni-Mn oxides, and fast and facile faradaic reactions on the electrode were responsible for the superior volumetric capacitance of 250 F cm-3 at 1 A cm-3, energy density as high as 22 mW h cm-3 and an excellent power density of 12 W cm-3. Despite the low CNT loading, the hybrid electrode exhibits excellent cycling performance with capacitance retention of 96.4% after 10 000 cycles evidencing a well-preserved Ni-manganese oxide nanostructure throughout the cycling. The resulting outstanding electrochemical performances of the Ni-Mn oxides/CNT@CNF synergic system offer new insights into effective utilization of transition metal oxides for establishing high-performance flexible supercapacitors within a confined volume.