Engineering 3‑D Li-Ion Electrodes with Enhanced Charge Storage Properties Based on Solution-Processed and Sintered Anatase Nanocrystal-Carbon Mesoporous Structures

Three-dimensional (3-D) monolithic electrodes are an excellent platform for enhancing the electrochemical properties of Li-ion batteries, but fabrication involves complex, difficult to scale-up processing. Current electrode fabrication based on polymeric binder-based pastes of the active material and carbon is expensive and requires volatile toxic organic solvents. Here, aqueous-synthesized anatase (∼6 nm) is used as active material in a green fabrication process employing controlled sintering at 450 °C of an ethanolic paste to engineer mesoporous 3-D structures. This enables construction of self-supporting electrodes endowed with a percolating carbon network with enhanced conductivity that exhibit highly stable cycling performance. As such, the new 3-D electrodes achieve greater capacity (185 vs 145 mAh g^–1 at 1C rate) than standard PVDF binder-based electrodes, and serve as a new approach toward easily scalable and sustainable electrode manufacturing applicable to various active materials