Nanoarchitectonics of lithium ion pathways through pores in a carbon framework for improving the storage capability and reversibility of lithium metal anode

• Published in: Applied organometallic chemistry Vol. 37; no. 10
• Main Authors: Han, Sang A, Suh, Joo Hyeong, Park, Min‐Sik, Kim, Jung Ho
• Format: Journal Article
• Language: English
• Published: Chichester Wiley Subscription Services, Inc 01-10-2023
• Subjects: Carbon; Channels; Chemistry; Degree of crystallinity; Electrical resistivity; Lithium; Lithium batteries; Lithium ions; lithium‐metal storage; Metal-organic frameworks; Metals; nanoporous carbon architecture; pyrolysis temperature; Storage; Structural stability; Surface stability; Zeolites; zeolitic imidazolate framework; Zinc
• ISSN: 0268-2605; 1099-0739
• DOI: 10.1002/aoc.7227

The utilization of lithium (Li) metal as an anode has attracted significant attention for high‐energy Li batteries. Unfortunately, uncontrollable Li dendrite cannot be avoided during Li plating and stripping. Much intensive research has been conducted to suppress the dendritic growth by confinement of metallic Li in host architectures. Recently, zeolitic imidazolate frameworks (ZIFs) with a porous features have been used to explore a new approach to storing the Li metal with the advantages of their structural and chemical stability, large surface areas, and large pore cavities. Herein, we investigate the storage capability of metallic Li in a porous carbon framework derived from ZIFs as a function of carbonization temperature. Diversities in pore volumes and channels, the degree of crystallinity, the amount of residual zinc (Zn) metal, and the electrical conductivity can all be controlled by temperature. We demonstrate that well‐connected pore channels and adequate electrical conductivity secure the Li‐ion pathways and that well‐distributed Zn clusters in porous carbon trigger the outward growth of metallic Li from inside the frameworks, resulting in a relatively low overpotential and long‐lasting cyclability. Our findings can provide practical insight into advanced electrode design for next‐generation Li metal batteries.
The inherent internal porosity of carbon frameworks derived from ZIF‐8 offers significant pathways for the efficient migration of Li‐ions and provides storage space. The presence of Zn clusters within the porous carbon structures aids in reducing the formation energy, thereby facilitating the growth of Li metal within the internal pores. The overpotential associated with the Li metallization reaction was effectively mitigated due to the low formation energy, ensuring excellent cycling stability by improving reversibility.