Developing multifunctional polymeric binders is key to the design of energy storage technologies with value-added features. We report that a multigram-scale synthesis of perylene diimide polymer (PPDI), from a single batch via polymer analogous reaction route, yields high molecular weight polymers with suitable thermal stability and minimized solubility in electrolytes, potentially leading to improved binding affinity toward electrode particles. Further, it develops strategies for designing copolymers with virtually any desired composition via a subsequent grafting, leading to purpose-built binders. PPDI dye as both binder and electroactive additive in lithium half-cells using lithium iron phosphate exhibits good electrochemical performance.

The commercial uptake of lithium-sulfur (Li-S) batteries is undermined by their rapid performance decay and short cycle life. These problems originate from the dissolution of lithium polysulfide in liquid electrolytes, causing charge and active material to shuttle between electrodes. The dynamics of intractable polysulfide migration at different length scales often tend to escape the probing ability of many analytical techniques. Spatial and temporal visualization of Li in Li-S electrodes and direct mechanistic understanding of how polysulfides are regulated across Li-S batteries starting from current collector and active layer coating to electrode-electrolyte interface are still lacking. To address this we employ neutron depth profiling across Li-S electrodes using the naturally occurring isotope, 6Li, which yields direct spatial information on Li-S electrochemistry. Using three types of Li-S electrodes, namely, carbon-sulfur, carbon-sulfur with 10% lithium titanium oxide (LTO), and carbon-sulfur with LTO membrane, we provide direct evidence for the migration, adsorption, and confinement of polysulfides in Li-S cells at work. Our findings further provide insights into the dynamics of polysulfide dissolution and re-utilization in relation to Li-S battery capacity and longevity to aid rational electrode designs toward high-energy, safe, and low-cost batteries.

Enabling the transition to renewable power sources requires further optimization of batteries in terms of energy/power density and cost-effectiveness. Increasing the practical thickness of Li ion battery electrodes not only can improve energy density on cell level but reduces manufacturing cost. However, thick electrodes exhibit sluggish charge-transport kinetics and are mechanically less stable, typically resulting in substandard battery performance compared to the current commercial standards (~50 μm). Here we disclose a novel method based on immersion precipitation by employing a non-solvent to solidify the battery binder, instead of solvent evaporation. This method allows for the fabrication of thick and suitable density electrodes (>100 μm with ultra-high mass loading) offering excellent electrochemical performance and mechanical stability. Using commercial electrode active materials at a remarkable mass-loading of 24 mg cm⁻², the electrodes processed via immersion method are shown to deliver 3.5 mAh cm⁻² at a rate of 2C and operate at rates up to 10C. As additional figure of merit, this method produces electrodes that are both stand-alone and highly flexible, which have been evaluated in flexible full-cells. Furthermore, via immersion precipitation the commonly used more toxic N-Methyl-2-pyrrolidone can be supplanted by environmentally benign dimethyl sulfoxide as solvent for processing electrode layers.