A Metal-Organic Framework Based Quasi-Solid-State Electrolyte Enabling Continuous Ion Transport for High-Safety and High-Energy-Density Lithium Metal Batteries.

Solid-state lithium metal batteries are promising next-generation rechargeable energy storage systems. However, the poor compatibility of the electrode/electrolyte interface and the low lithium ion conductivity of solid-state electrolytes are key issues hindering the practicality of solid-state electrolytes. Herein, rational designed metal-organic frameworks (MOFs) with the incorporation of two types of ionic liquids (ILs) are fabricated as quasi-solid electrolytes. The obtained MOF-IL electrolytes offer continuous ion transport channels with the functional sulfonic acid groups serving as lithium ion hopping sites, which accelerate the Li+ transport both in the bulk and at the interfaces. The quasi-solid MOF-IL electrolytes exhibit competitive ionic conductivities of over 3.0 × 10-4 S cm-1 at room temperature, wide electrochemical windows over 5.2 V, and good interfacial compatibility, together with greatly enhanced Li+ transference numbers compared to the bare IL electrolyte. Consequently, the assembled quasi-solid Li metal batteries show either superior stability at low C rates or improved rate performance, related to the species of ILs. Overall, the quasi-solid MOF-IL electrolytes possess great application potential in high-safety and high-energy-density lithium metal batteries.

Graphdiyne-like Porous Organic Framework as a Solid-Phase Sulfur Conversion Cathodic Host for Stable Li-S Batteries.

As a unique branch of Li-S batteries, solid-phase sulfur conversion polymer cathodes have shown superior stability with fast ion-transfer kinetics and high discharge capacities owing to the mere existence of short-chain sulfur species during charging/discharging. However, representative compounds such as sulfurized polyacrylonitrile (SPAN) and polyaniline (SPANI) suffer from low sulfur contents and poor cycling performances under large current densities due to the sulfurization occurring only on polymers' surface. Here, a graphdiyne-like porous organic framework, denoted as GPOF, is synthesized and used as a host for enabling solid-phase sulfur conversion. Plenty of unsaturated bonds in GPOF provide sufficient reaction sites to bind sulfur chains, resulting in a high active sulfur content in the cathode. Moreover, the microporous GPOF possesses suitable cavities to accommodate the volume expansion, leading to favorable long-term cycling stability. As a result, the sulfurized GPOF cathode (SGPOF-320) displays outstanding electrochemical stability with negligible capacity decline after 250 cycles at 0.2 C with an average discharge capacity of 925 mA h g-1. Our work applies a facile procedure to produce sulfur conversion porous polymer cathodes, which could provide a proper way for exploring more suitable cathode materials for high-performance Li-S batteries.