A facile solvothermal polymerization approach to thermoplastic polymer-based nanocomposites as alternative anodes for high-performance lithium-ion batteries

Zongfeng Sha, Shengqiang Qiu, Qing Zhang, Zhiyong Huang, Xun Cui, Yingkui Yang, Zhiqun Lin

Research output: Contribution to journalArticlepeer-review

24 Scopus citations


Conventional inorganic electrode materials for lithium-ion batteries (LIBs) face inherent limitations in electrochemical performance, natural resources, environmental issues, mechanical robustness, and cost. Organic redox polymers have recently attracted considerable attention as potential low-cost alternative electrodes for green LIBs; however, they are often employed as cathode materials. Herein a simple one-pot solvothermal polymerization approach was developed to produce graphene/chemically crosslinked poly(methyl methacrylate) (Gr/c-PMMA) composites as robust anodes for high-performance LIBs. As control samples, linear PMMA and pure c-PMMA are also solvothermally polymerized without and with the addition of a crosslinker, respectively, in the absence of graphene oxide. Such thermoplastic PMMA-based materials as anodes for LIBs exhibit a pair of stable redox peaks at 0.79 and 1.02 V over a potential range of 0.01 to 2.5 V, due to their highly reversible lithiation/delithiation of the in situ generated 1,2-cyclopentanedione active units. The reversible capacities of PMMA, c-PMMA, and Gr/c-PMMA anodes are 97, 147, and 206 mA h g-1 at 20 mA g-1, respectively. After increasing to 400 mA g-1, the Gr/c-PMMA anode manifests a capacity retention of 82%, higher than those of c-PMMA (72%) and PMMA (38%) anodes. Moreover, Gr/c-PMMA delivers a high capacity of 159 mA h g-1 after 1000 cycles at 400 mA g-1. Notably, compared to PMMA, the better performance of c-PMMA can be attributable to the chemical crosslinking induced-formation of porous networks consisting of smaller nanoparticles (∼50 nm) for c-PMMA than those of PMMA (∼100 nm). The incorporation of uniformly dispersed graphene into c-PMMA enables the creation of 3D conductive networks with interconnected porous channels, thereby providing the efficient electrochemical activity of Gr/c-PMMA while retaining the structural integrity during cycling. This, in turn, results in a large specific capacity, a high rate capability, and a long-term cycling stability. These findings may provide new insights into the exploration of low-cost commercial plastics for rechargeable batteries as well as the possibility of other high added-value energy applications by capitalizing on recyclable plastics.

Original languageEnglish
Pages (from-to)23019-23027
Number of pages9
JournalJournal of Materials Chemistry A
Issue number40
StatePublished - 2019

Bibliographical note

Funding Information:
This work was supported by the National Natural Science Foundation of China (Grants 51673061 and 51973235) and the Fundamental Research Funds for the Central Universities (Grants CZP19001 and CZQ19003).

Publisher Copyright:
© The Royal Society of Chemistry 2019.


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