Ultra-Thin Hydrogen-Organic-Framework (HOF) Nanosheets for Ultra-Stable Alkali Ions Battery Storage

Organic frameworks-based batteries with excellent physicochemical stability and long-term high capacity will definitely reduce the cost, carbon emissions, and metal consumption and contamination. Here, an ultra-stable and ultra-thin perylene-dicyandiamide-based hydrogen organic framework (HOF) nanosheet (P-DCD) of approximate to 3.5 nm in thickness is developed. When applied in the cathode, the P-DCD exhibits exceptional long-term capacity retention for alkali-ion batteries (AIBs). Strikingly, for lithium-ion batteries (LIBs), at current of 2 A g(-1), the large reversible capacity of 108 mA h g(-1) shows no attenuation within 5 000 cycles. For sodium-ion batteries (SIBs), the related capacity retains 91.7% within 10 000 cycles compared to the initial state, significantly much more stable than conventional organic materials reported previously. Mechanism studies through ex situ and in situ experiments and theoretical density functional theory (DFT) calculations reveal that the impressive long-term performance retention originates from the large electron delocalization, fast ion diffusion, and physicochemical stability within the ultra-thin 2D P-DCD, featuring pi-pi and hydrogen bonding stacking, nitrogen-rich units, and low impedance. The advantageous features demonstrate that rationally designed stable and effective organic frameworks pave the way to utilizing complete organic materials for developing next-generation low-cost and highly stable energy storage batteries.

Automated summary

This study develops an ultra-stable and ultra-thin hydrogen organic framework nanosheet with exceptional long-term capacity retention in lithium-ion and sodium-ion batteries. Mechanism studies reveal that the impressive performance retention is attributed to large electron delocalization, fast ion diffusion, and physicochemical stability within the nanosheet. The advantageous features pave the way for developing next-generation low-cost and highly stable energy storage batteries.