Expansion-tolerant architectures for stable cycling of ultrahigh-loading sulfur cathodes in lithium-sulfur batteries

Lithium-sulfur batteries can displace lithium-ion by delivering higher specific energy. Presently, however, the superior energy performance fades rapidly when the sulfur electrode is loaded to the required levels—5 to 10 mg cm(−2)— due to substantial volume change of lithiation/delithiation and the resultant stresses. Inspired by the classical approaches in particle agglomeration theories, we found an approach that places minimum amounts of a high-modulus binder between neighboring particles, leaving increased space for material expansion and ion diffusion. These expansion-tolerant electrodes with loadings up to 15 mg cm(−2) yield high gravimetric (>1200 mA·hour g(−1)) and areal (19 mA·hour cm(−2)) capacities. The cells are stable for more than 200 cycles, unprecedented in such thick cathodes, with Coulombic efficiency above 99%.