Creating Vacancy Strong Interaction to Enable Homogeneous High‐Throughput Ion Transport for Efficient Solid‐State Lithium Batteries

Ya Song; Haotian Qu; Zhoujie Lao; Xiao Xiao; Yanze Song; Lu Nie; Jian Wang; Jinlong Yang; Yanfei Zhu; Guangmin Zhou

doi:10.1002/adma.202419271

journal article Mar 23, 2025

Creating Vacancy Strong Interaction to Enable Homogeneous High‐Throughput Ion Transport for Efficient Solid‐State Lithium Batteries

Ya Song

Haotian Qu

Zhoujie Lao Xiao Xiao

Yanze Song Lu Nie Jian Wang

Jinlong Yang

Yanfei Zhu Guangmin Zhou

Advanced Materials Vol. 37 No. 18 · Wiley

View at Publisher Save 10.1002/adma.202419271

Abstract

AbstractSolid polymer electrolytes are emerging as a key component for solid‐state lithium metal batteries, offering a promising combination of large‐scale processability and high safety. However, challenges remain, including limited ion transport and the unstable solid electrolyte interphase, which result in unsatisfactory ionic conductivity and uncontrollable lithium dendrite growth. To address these issues, a high‐throughput Li‐ion transport pathway is developed by incorporating tungsten sulfide enriched with sulfur vacancies (SVs) into a poly(vinylidene fluoride‐co‐hexafluoropropylene)‐based composite polymer electrolytes (CPEs). The SVs strong interaction in the CPEs facilitates homogeneous high‐throughput Li‐ion transport 1.9 × 10−3 S cm−1 at 25 °C) by enhancing the dissociation of lithium salts and effectively creates ample interfaces with the polymer chains to reduce the formation of inner vacuities. Moreover, the SVs confine FSI− anions, while the electron‐rich environment induced by sulfur atoms promotes the preferential degradation of bis(trifluoromethanesulfonyl)imide anions, ensuring uniform lithium deposition. This fosters the formation of inorganic nanocrystals on the lithium anode and effectively suppresses dendrite growth, enabling an ultra‐long lifetime of over 5500 h in Li||Li symmetric cells. When paired with sulfurized polyacrylonitrile cathode, a pouch cell capacity of 0.524 Ah is achieved, demonstrating the effectiveness of a homogeneous, high‐throughput Li‐ions transport mechanism.

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References

Details

Published: Mar 23, 2025
Vol/Issue: 37(18)
License: View

Authors

Y

Ya Song

Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 China; Guangdong Provincial Key Laboratory of New Energy Materials Service Safety College of Materials Science and Engineering Shenzhen University Shenzhen 518060 China

H

Haotian Qu

Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 China

Z

Zhoujie Lao

Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 China

X

Xiao Xiao

Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 China

Y

Yanze Song

Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 China

L

Lu Nie

Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 China

J

Jian Wang

Canadian Light Source Saskatoon S7N 2V3 Canada

J

Jinlong Yang

Guangdong Provincial Key Laboratory of New Energy Materials Service Safety College of Materials Science and Engineering Shenzhen University Shenzhen 518060 China

Y

Yanfei Zhu

Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 China

G

Guangmin Zhou

Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 China

Funding

National Natural Science Foundation of China Award: U21A20174

Guangdong Innovative and Entrepreneurial Research Team Program Award: 2021ZT09L197

National Key Research and Development Program of China Award: 2021YFB2500200

Shenzhen Science and Technology Innovation Program Award: KQTD20210811090112002

Cite This Article

Ya Song, Haotian Qu, Zhoujie Lao, et al. (2025). Creating Vacancy Strong Interaction to Enable Homogeneous High‐Throughput Ion Transport for Efficient Solid‐State Lithium Batteries. Advanced Materials, 37(18). https://doi.org/10.1002/adma.202419271

Creating Vacancy Strong Interaction to Enable Homogeneous High‐Throughput Ion Transport for Efficient Solid‐State Lithium Batteries

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