Highly stable multi-layered silicon-intercalated graphene anodes for lithium-ion batteries

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Research Letter

Highly stable multi-layered silicon-intercalated graphene anodes for lithium-ion batteries Doyoung Kim, Centre for Integrated Nanostructure Physics (CINAP), Institute for Basic Science (IBS), Sungkyunkwan University, Suwon 16419, Republic of Korea; Department of Energy Science, Sungkyunkwan University, Suwon 16419, Republic of Korea Yongguang Luo, Department of Chemistry, Sungkyunkwan University, Suwon 16419, Republic of Korea Anand P. Tiwari, Department of Material Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea Hee Min Hwang and Simgeon Oh, Centre for Integrated Nanostructure Physics (CINAP), Institute for Basic Science (IBS), Sungkyunkwan University, Suwon 16419, Republic of Korea; Department of Energy Science, Sungkyunkwan University, Suwon 16419, Republic of Korea Keunsik Lee , Department of Chemistry, Sungkyunkwan University, Suwon 16419, Republic of Korea Hyoyoung Lee , Centre for Integrated Nanostructure Physics (CINAP), Institute for Basic Science (IBS), Sungkyunkwan University, Suwon 16419, Republic of Korea; Department of Energy Science, Sungkyunkwan University, Suwon 16419, Republic of Korea; Department of Chemistry, Sungkyunkwan University, Suwon 16419, Republic of Korea Address all correspondence to Hyoyoung Lee at [email protected] (Received 23 November 2019; accepted 12 February 2020)

Abstract To avoid degradation of silicon anodes in lithium-ion batteries (LIBs), the authors report a new two-dimensional multi-layered Si-intercalated rGO (rGO/Si) anode prepared by direct growth of Si into a porous multi-layered reduced graphene oxide (rGO) film. Direct Si deposition onto the porous rGO film allows the Si layers to be intercalated into the film via in situ replacement of the oxygen groups of the multi-layered graphene oxide (GO) with Si through thermal reduction of the GO film. The porous rGO acts as a cushion against the expansion of the Si layer during lithiation, preventing the Si from being pulverized and producing highly stable LIBs.

Introduction With the development of portable devices and electric vehicles, the development of lithium-ion batteries (LIBs) with higher energy capacity and longer cycle stability has become necessary.[1] Silicon (Si)-derivative anode materials have shown the highest theoretical capacity (4200 mAh/g) and have garnered much interest.[2] However, when using Si materials in LIBs, a few critical problems are encountered, such as a low electrical conductivity, volume expansion (∼400%), and pulverization of Si during Li-ion insertion and deinsertion into the Si layer.[3] The volume expansion and pulverization problems lead to capacity fading, causing pulverization of the anodes. Previous studies using bulk and micro-sized Si show high capacity values at the onset but large fading as the number of cycles increased.[4] This is caused by the destruction of the structure due to expansion and pulverization of Si that accompanies the lithiation and delithiation processes and ultimately reduces s