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Nano Research 2023, 16(10): 12304-12314 https://doi.org/10.1007/s12274-023-5947-9
Research Article | Issue | Published: 08 August 2023

Laser irradiation constructing all-in-one defective graphene-polyimide separator for effective restraint of lithium dendrites and shuttle effect

Show Author's Information Jiawei Mu1,§,  Mengdi Zhang1,§( ),  Yanan Li1,  Zhiliang Dong1,  Yuanyuan Pan2,  Bei Chen1,  Zhengqiu He1,  Haiqiu Fang1,  Shuoshuo Kong1,  Xin Gu1,  Han Hu1,  Mingbo Wu1( )
State Key Laboratory of Heavy Oil Processing, Advanced Chemical Engineering and Energy Materials Research Center, College of New Energy, China University of Petroleum (East China), Qingdao 266580, China
College of Physics, University-Industry Joint Center for Ocean Observation and Broadband Communication, State Key Laboratory of Bio-Fibers and Eco Textiles, Qingdao University, Qingdao 266071, China

§ Jiawei Mu and Mengdi Zhang contributed equally to this work.

Keywords:
lithium-sulfur batteries, laser-induced graphene, shuttle effect, Li dendrites, separators, intrinsic carbon defects
Topics:
Lithium sulfur batteries
Cite this article:
Mu J, Zhang M, Li Y, et al. Laser irradiation constructing all-in-one defective graphene-polyimide separator for effective restraint of lithium dendrites and shuttle effect. Nano Research, 2023, 16(10): 12304-12314. https://doi.org/10.1007/s12274-023-5947-9
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Abstract Full text Electronic supplementary material About this article

The commercialization of lithium-sulfur (Li-S) batteries faces several bottlenecks, and the major two of which are the shuttle effect of polysulfides and the wild growth of Li dendrites, responsible for fast capacity decay and severe safety issues. As an essential component of Li-S batteries, the structure and properties of the separators are closely related to the above problems, and the exploration of multifunctional separators is highly sought-after. Herein, an integrated separator composited of defective graphene and polyimide (DG-PI) was innovatively fabricated by electrospinning combined with the laser-induced carbonization strategy. The all-in-one compact architecture with well-interconnected channels shows superior mechanical and thermal stability and wettability. More importantly, the PI nanofibers containing N–/O– functional groups can induce the uniform deposition of lithium on the anode surface, while the DG framework with abundant pentagonal/heptagonal rings and vacancies can strongly trap polysulfides and accelerate polysulfide transformation on the cathode side. The strong chemical interaction between the insulative PI layer and the conductive DG layer modulates the surface charge distribution of each other, leading to more prominent contributions to restraining lithium dendrites and shuttle effect. Therefore, the Li-S batteries based on the integrated DG-PI separators afford an excellent performance in protecting lithium anode (stable cycles of 200 h at 5 mA·cm−2) and good cycling stability with a low capacity decay of 0.05% per cycle after 700 cycles at 1 C. This work offers a new design concept of multifunctional Li-S battery separators and broadens the application scope of laser micro-nano fabrication technology.


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Electronic supplementary material
About this article

Laser irradiation constructing all-in-one defective graphene-polyimide separator for effective restraint of lithium dendrites and shuttle effect

Show Author's information Jiawei Mu1,§, Mengdi Zhang1,§( ), Yanan Li1, Zhiliang Dong1, Yuanyuan Pan2, Bei Chen1, Zhengqiu He1, Haiqiu Fang1, Shuoshuo Kong1, Xin Gu1, Han Hu1, Mingbo Wu1( )
State Key Laboratory of Heavy Oil Processing, Advanced Chemical Engineering and Energy Materials Research Center, College of New Energy, China University of Petroleum (East China), Qingdao 266580, China
College of Physics, University-Industry Joint Center for Ocean Observation and Broadband Communication, State Key Laboratory of Bio-Fibers and Eco Textiles, Qingdao University, Qingdao 266071, China

§ Jiawei Mu and Mengdi Zhang contributed equally to this work.

Abstract

The commercialization of lithium-sulfur (Li-S) batteries faces several bottlenecks, and the major two of which are the shuttle effect of polysulfides and the wild growth of Li dendrites, responsible for fast capacity decay and severe safety issues. As an essential component of Li-S batteries, the structure and properties of the separators are closely related to the above problems, and the exploration of multifunctional separators is highly sought-after. Herein, an integrated separator composited of defective graphene and polyimide (DG-PI) was innovatively fabricated by electrospinning combined with the laser-induced carbonization strategy. The all-in-one compact architecture with well-interconnected channels shows superior mechanical and thermal stability and wettability. More importantly, the PI nanofibers containing N–/O– functional groups can induce the uniform deposition of lithium on the anode surface, while the DG framework with abundant pentagonal/heptagonal rings and vacancies can strongly trap polysulfides and accelerate polysulfide transformation on the cathode side. The strong chemical interaction between the insulative PI layer and the conductive DG layer modulates the surface charge distribution of each other, leading to more prominent contributions to restraining lithium dendrites and shuttle effect. Therefore, the Li-S batteries based on the integrated DG-PI separators afford an excellent performance in protecting lithium anode (stable cycles of 200 h at 5 mA·cm−2) and good cycling stability with a low capacity decay of 0.05% per cycle after 700 cycles at 1 C. This work offers a new design concept of multifunctional Li-S battery separators and broadens the application scope of laser micro-nano fabrication technology.

Keywords: lithium-sulfur batteries, laser-induced graphene, shuttle effect, Li dendrites, separators, intrinsic carbon defects

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Publication history
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Acknowledgements

Publication history

Received: 01 March 2023
Revised: 09 June 2023
Accepted: 21 June 2023
Published: 08 August 2023
Issue date: October 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 22005341 and 22138013), the Shandong Provincial Natural Science Foundation (Nos. ZR2020QB128 and ZR2020ZD08), the Taishan Scholar Project (No. tsqnz20221121), the Major Scientific and Technological Innovation Project of Shandong Province (No. 2020CXGC010402), and the Independent Innovation Research Project of China University of Petroleum (No. 22CX06026A).

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