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Research Article

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

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.

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Graphical Abstract

An all-in-one separator integrating defect-rich graphene framework with polyimide nanofibers is proposed for the first time to restrain lithium dendrites and shuttle effect simultaneously, thus enabling excellent electrochemical performances and safety of Li-S batteries.

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 batteriesseparatorslaser-induced grapheneintrinsic carbon defectsshuttle effectLi dendrites

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Nano Research
Volume 16 Issue 10,
October 2023
Pages 12304-12314
DOI: 10.1007/s12274-023-5947-9
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
Topics:
Lithium sulfur batteries
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Received: 01 March 2023
Revised: 09 June 2023
Accepted: 21 June 2023
Published: 08 August 2023
© Tsinghua University Press 2023
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