The hierarchical porous structure has garnered considerable attention as a multiscale engineering strategy to bring unforeseen synergistic effects in a vast variety of functional materials. Here, we demonstrate a "microporous covalent organic framework (COF) net on mesoporous carbon nanotube (CNT) net" hybrid architecture as a new class of molecularly designed, hierarchical porous chemical trap for lithium polysulfides (Li2Sx) in Li-S batteries. As a proof of concept for the hybrid architecture, self-standing COF-net on CNT-net interlayers (called "NN interlayers") are fabricated through CNT-templated in situ COF synthesis and then inserted between sulfur cathodes and separators. Two COFs with different micropore sizes (COF-1 (0.7 nm) and COF-5 (2.7 nm)) are chosen as model systems. The effects of the pore size and (boron-mediated) chemical affinity of microporous COF nets on Li2Sx adsorption phenomena are theoretically investigated through density functional theory calculations. Benefiting from the chemical/structural uniqueness, the NN interlayers effectively capture Li2Sx without impairing their ion/electron conduction. Notably, the COF-1 NN interlayer, driven by the well-designed microporous structure, allows for the selective deposition/dissolution (i.e., facile solid-liquid conversion) of electrically inert Li2S. As a consequence, the COF-1 NN interlayer provides a significant improvement in the electrochemical performance of Li-S cells (capacity retention after 300 cycles (at charge/discharge rate = 2.0 C/2.0 C) = 84% versus 15% for a control cell with no interlayer) that lies far beyond those accessible with conventional Li-S technologies.

The flexible/shape-versatile bipolar all-solid-state LIBs, which fabricated via solvent-drying-free, UV-curing-assisted multistage printing, are presented as an unprecedented material/process strategy to address longstanding challenges associated with inorganic-electrolyte-based bipolar LIBs.

) of long-range (=300 miles) electric vehicle batteries. In addition, the heteronet-enabled mechanical compliance of CM electrodes, in combination with readily deformable CNF separators, allows the fabrication of paper crane batteries via origami folding technique.

Recent developments of non-covalent functionalization of carbon nanotubes (CNTs) require a systematic understanding of the interaction between molecule and CNTs (CNT-molecular interaction); however, it has been difficult to evaluate the "net" interaction between the CNTs and molecules. We now use silica gel particles coated with the pristine single-walled carbon nanotubes (SWNTs) in a monolayer fashion as the stationary phase of a HPLC column. The newly developed column (SWNT-column) worked as a powerful tool for ranking the interactions between the SWNTs and molecules with a high precision. We describe the binding affinity analysis of polyaromatic hydrocarbons onto the surfaces of SWNTs. The obtained ranking is determined in the order of benzene < naphthalene < biphenyl < fluorene < phenanthrene < anthracene ∼ pyrene < triphenylene < p-terphenyl < tetraphene < tetracene.

Spiderweb‐mimicking anion‐exchangeable separators are presented as a membrane‐driven strategy for the development of high‐performance Li‐S batteries by Sang‐Young Lee and co‐workers in article number https://doi.org/10.1002/adfm.201801422. The polyionic liquid (PVIm[TFSI])‐based nanomat in the spider separator enables discharge voltage‐dependent, reversible trap/release of polysulfides via an anion exchange reaction between TFSI− anions and polysulfides. The seperator's unique nanomat structure and chemical functionalities exceptionally improve the electrochemical performance of Li‐S batteries.