DOE OSTI · 3376743
Superionic Surface Li-Ion Transport in Carbonaceous Materials
Abstract
Unlike Li-ion transport in the bulk of carbonaceous materials, little is known about Li-ion diffusion on their surface. Here, in this study, we have discovered an ultrafast Li-ion transport phenomenon on the surface of carbonaceous materials with limited reversible Li insertion capacity and high surface area. An ionic conductivity of 18.1 mS cm –1 at room temperature is observed in lithiated Ketjen black (KB), far exceeding those of most solid-state ion conductors. Theoretical calculations reveal low diffusion barriers for the surface Li species. As a result, lithiated KB functions effectively as an interlayer between Li and solid-state electrolytes (SSEs) to mitigate dendrite growth. Further, lithiated KB acts as a high-performance mixed ionic–electronic conductor and replaces solid electrolytes to enhance graphite anode performance, demonstrating full utilization with ∼85% capacity retention over 300 cycles. The discovery of this surface-mediated ultrafast Li-ion transport mechanism provides new directions for the design of solid-state ion conductors and solid-state batteries.
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Zhou, Jianbin [Univ. of California, San Diego, CA (United States)], Wang, Shen [Univ. of California, San Diego, CA (United States)], Wu, Chaoshan [Univ. of Houston, TX (United States)], Qi, Ji [Univ. of California, San Diego, CA (United States)] (ORCID:0000000158089931), Wan, Hongli [Univ. of Maryland, College Park, MD (United States)], Lai, Shen [Univ. of California, San Diego, CA (United States)], Ko, Tsz Wai [Univ. of California, San Diego, CA (United States)], Liang, Zhaohui [Univ. of California, San Diego, CA (United States)], Feng, Shijie [Univ. of California, San Diego, CA (United States)] (ORCID:0000000157978542), Zhou, Ke [Univ. of California, San Diego, CA (United States)], Harpak, Nimrod [Univ. of California, San Diego, CA (United States)], Liu, Mengchen [Univ. of California, San Diego, CA (United States)], Hui, Zeyu [Univ. of California, San Diego, CA (United States)], Ai, Paulina J. [The Bishop’s School, La Jolla, CA (United States)], Liu, Haodong [Univ. of California, San Diego, CA (United States)], Yan, Wenlin [Univ. of California, San Diego, CA (United States)], Ha, Yang [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000156848420), Kim, Min-Jae [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)], Griffith, Kent [Univ. of California, San Diego, CA (United States)] (ORCID:000000028096906X), Wang, Chunsheng [Univ. of Maryland, College Park, MD (United States)] (ORCID:0000000286266381), Ong, Shyue Ping [Univ. of California, San Diego, CA (United States)] (ORCID:0000000157262587), Yao, Yan [Univ. of Houston, TX (United States)], Liu, Ping [Univ. of California, San Diego, CA (United States)] (ORCID:0000000214881668). 2025-08-15. Superionic Surface Li-Ion Transport in Carbonaceous Materials. https://doi.org/10.1021/acs.nanolett.5c02729
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