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

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Ultra-Thin Hydrogen-Organic-Framework (HOF) Nanosheets for Ultra-Stable Alkali Ions Battery Storage
Small ( IF 13.0 ) Pub Date : 2023-11-10 , DOI: 10.1002/smll.202307827
Jialong Tang ₁ , Ruoxuan Yang ₁ , Yuting Peng ₁ , Hong Lin ₁ , Xin He ₁ , Yingze Song ₁ , Kaipeng Wu ₂ , Youngsoo Kang ₃ , Long Yang _{1,

3}

Affiliation

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 ≈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 π-π 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.

中文翻译：

用于超稳定碱离子电池存储的超薄氢有机框架（HOF）纳米片

有机骨架电池具有优异的物理化学稳定性和长期高容量，必将降低成本、碳排放、金属消耗和污染。在此，开发了厚度约3.5 nm的超稳定、超薄苝-双氰胺基氢有机骨架（HOF）纳米片（P-DCD）。当应用于阴极时，P-DCD 对碱离子电池 (AIB) 表现出卓越的长期容量保持能力。引人注目的是，对于锂离子电池（LIB），在2 A g ^-1电流下，108 mA hg ^-1的大可逆容量在5 000次循环内没有表现出衰减。对于钠离子电池（SIB），与初始状态相比，在10000次循环内相关容量保留了91.7%，比之前报道的传统有机材料稳定得多。通过异位和原位实验以及理论密度泛函理论 (DFT) 计算进行的机理研究表明，令人印象深刻的长期性能保持源于超薄 2D P-DCD 内的大电子离域、快速离子扩散和物理化学稳定性，具有π-π和氢键堆积、富氮单元和低阻抗等特点。这些优势特征表明，合理设计的稳定有效的有机框架为利用完全有机材料开发下一代低成本和高稳定性储能电池铺平了道路。

更新日期：2023-11-10

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