Stepped Channels Integrated Lithium–Sulfur Separator via Photoinduced Multidimensional Fabrication of Metal–Organic Frameworks

Multidimensional fabrication of metal–organic frameworks (MOFs) into multilevel channel integrated devices are in high demanded for Li‐S separators. Such separators have advantages in pore‐engineering that might fulfill requirements such as intercepting the diffusing polysulfides and improving the Li+/electrolyte transfer in Li‐S batteries. However, most reported works focus on the roles of MOFs as ionic sieves for polysulfides while offering limited investigation on the tuning of Li+ transfer across the separators. A photoinduced heat‐assisted processing strategy is proposed to fabricate MOFs into multidimensional devices (e.g., hollow/Janus fibers, double‐or triple‐layer membranes). For the first time, a triple‐layer separator with stepped‐channels has been designed and demonstrated as a powerful separator with outstanding specific capacity (1365.0 mAh g−1) and cycling performance (0.03 % fading per cycle from 100th to 700th cycle), which is superior to single/double‐layer and commercial separators. The findings may expedite the development of MOF‐based membranes and extend the scope of MOFs in energy‐storage technologies. A two‐step photoinduced heat‐assisted processing (PHAP) method is proposed to fabricate a kind of metal–organic framework (MOF)‐based triple‐layer membrane with stepped channels. The membrane can be applied as a high performance separator in a lithium–sulfur battery.