Grain‐Boundary‐Rich Triphasic Artificial Hybrid Interphase Toward Practical Magnesium Metal Anodes

Grain‐Boundary‐Rich Triphasic Artificial Hybrid Interphase Toward Practical Magnesium Metal Anodes

Advanced Functional Materials

10.1002/adfm.202210639

http://dx.doi.org/10.1002/adfm.202210639

Yuanjian Li, Gaoliang Yang, Chang Zhang, Wei Ying Lieu, Carina Yi Jing Lim, Shengnan Sun, Jianbiao Wang, Shunqiong Jiang, Zhenxiang Xing, Zdenek Sofer, Man‐Fai Ng, Wei Liu, Zhi Wei Seh

Biomaterials, Electrochemistry, Electronic, Optical and Magnetic Materials, Condensed Matter Physics

20 November 2022

Li, Y., Yang, G., Zhang, C., Lieu, W. Y., Lim, C. Y. J., Sun, S., Wang, J., Jiang, S., Xing, Z., Sofer, Z., Ng, M., Liu, W., & Seh, Z. W. (2022). Grain‐Boundary‐Rich Triphasic Artificial Hybrid Interphase Toward Practical Magnesium Metal Anodes. Advanced Functional Materials, 33(5), 2210639. Portico. https://doi.org/10.1002/adfm.202210639

Magnesium metal anodes have attracted widespread attention for their high volumetric capacity and natural abundance, but are precluded from practical applications by poor rate capability and limited lifespan due to sluggish ion-transfer kinetics and uneven deposition behavior. Herein, for the first time a grain-boundary-rich triphasic artificial hybrid interphase, consisting of Sb metal, Mg3Sb2 alloy, and MgCl2, is designed on Mg anode surface by a facile solution treatment method, enabling high-rate and long-cycle Mg plating/stripping behavior. The triphasic artificial hybrid interphase affords high magnesiophilicity and ionic conductivity to reduce the energy barriers for Mg2+ desolvation and deposition. Meanwhile, the abundant grain boundaries redistribute Mg2+ flux at the electrode-electrolyte interface and guide uniform Mg deposition. Accordingly, the as-designed Mg metal anode achieves ultralong cycling life of 350 h at a high current density of 5 mA cm−2 and a large areal capacity of 5 mAh cm−2, outperforming previously reported Mg metal anodes with artificial interphases. Full cells with Mo6 cathode also show extraordinary stability over a long lifespan of 8000 cycles at a high rate of 5 C. The rational artificial interphase design and the understanding of composition-structure-function relationships shed deep insights into the development of fast-charging and long-cycling Mg metal batteries.

Publisher Copyright

This research is supported by core funding from: SERC
Grant Reference no. : NA

The Czech Science Foundation (GACR no. 20-16124J)

This is the peer reviewed version of the following article: Li, Y., Yang, G., Zhang, C., Lieu, W. Y., Lim, C. Y. J., Sun, S., Wang, J., Jiang, S., Xing, Z., Sofer, Z., Ng, M., Liu, W., & Seh, Z. W. (2022). Grain‐Boundary‐Rich Triphasic Artificial Hybrid Interphase Toward Practical Magnesium Metal Anodes. Advanced Functional Materials, 33(5), 2210639. Portico. https://doi.org/10.1002/adfm.202210639, which has been published in final form at doi.org/10.1002/adfm.202210639. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.

https://oar.a-star.edu.sg/communities-collections/articles/19141

1616-3028
1616-301X

Institute of Materials Research and Engineering