Reconstructable Carbon Monolayer-MoS2 Intercalated Heterostructure Enabled by Atomic Layers-Confined Topotactic Transformation for Ultrafast Lithium Storage

Kexuan Liao; Lu Chen; Ruijin Meng; Yutong Feng; Shuo Meng; Hang Lu; Jie Ma; Chengxin Peng; Chi Zhang; Jinhu Yang

doi:10.1021/jacs.4c01550

Reconstructable Carbon Monolayer-MoS₂ Intercalated Heterostructure Enabled by Atomic Layers-Confined Topotactic Transformation for Ultrafast Lithium Storage

J Am Chem Soc. 2024 May 1;146(17):12020-12029. doi: 10.1021/jacs.4c01550. Epub 2024 Apr 23.

Authors

Kexuan Liao^{1

2}, Lu Chen^{1

2}, Ruijin Meng³, Yutong Feng¹, Shuo Meng¹, Hang Lu¹, Jie Ma⁴, Chengxin Peng⁵, Chi Zhang^{1

2}, Jinhu Yang^{1

2}

Affiliations

¹ School of Chemical Science and Engineering, Tongji University, Shanghai 200092, P. R. China.
² State Key Laboratory of Cardiovascular Diseases, Shanghai East Hospital, School of Medicine, Tongji University, Shanghai 200092, P. R. China.
³ Department of Applied Physics, The Hong Kong Polytechnic University, Hunghom 999077, Hong Kong.
⁴ College of Environmental Science and Engineering, Tongji University, Siping Road 1239, Shanghai 200092, P. R. China.
⁵ School of Materials and Chemistry, University of Shanghai for Science and Technology, Shanghai 200093, P. R. China.

PMID: 38651300
DOI: 10.1021/jacs.4c01550

Abstract

The intercalation structure of two-dimensional materials with expanded interlayer distance can facilitate mass transport, which is promising in fast-charging lithium-ion batteries (LIBs). However, the designed intercalation structures will be pulverized and destroyed under tough working conditions, causing overall performance deterioration of the batteries. Here, we present that an intercalated heterostructure made of the typical layered material of MoS₂ intercalated by N-doped graphene-like carbon monolayer (MoS₂/g-CM) through a polymer intercalation strategy exhibits a unique behavior of reversible reconstructability as an LIB anode during cycling. A mechanism of "carbon monolayers-confined topotactic transformation" is proposed, which is evidenced by substantial in/ex situ characterizations. The intercalated heterostructure of MoS₂/g-CM featuring a reconstructable property and efficient interlayer electron/ion transport exhibits an unprecedented rate capability up to 50 A g^-1 and outstanding long cyclability. Moreover, the proposed strategy based on g-CM intercalation has been extended to the MoSe₂ system, also realizing reconstructability of the intercalated heterostructure and improved LIB performance, demonstrating its versatility and great potential in applications.