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Chem. J. Chinese Universities

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In-situ Construction of a Stable N-doped Graphene/Carbon Nanotubes Three-dimensional Host for Dendrite-free and Long-life Lithium Metal Anodes

SHE Suhui1,2，XIN Guoxiang1,2*，BAO Jinxiao1,2*，SUN Guangshu1,2，WANG Haitao3，SONG Jinling1,2，WANG Qingchun1,2，BULIN Chaoke1,2，ZHANG Jinhui4*   

  1. 1. School of Materials Science and Engineering, Inner Mongolia Key Laboratory of Advanced Ceramic Material and Devices, Inner Mongolia University of Science and Technology 2. Key Laboratory of Green Extraction & Efficient Utilization of Light Rare-Earth Resources(Inner Mongolia University of Science and Technology), Ministry of Education 3.Hunan Keba automotive power battery Co., Ltd. Beijing Branch 4.School of New Materials and Chemical Engineering, Tangshan University
  • Received:2026-04-20 Revised:2026-05-30 Online First:2026-06-01 Published:2026-06-01
  • Contact: Guo-Xiang XIN E-mail:xinguoxiang@imust.edu.cn
  • Supported by:
    Supported by the the National Natural Science Foundation of China(Nos.52362035, 22462023), the Basic Research Funds for Universities Directly under Inner Mongolia Autonomous Region, China(No.2023QNJS018), the Science and Technology Breakthrough Project of Inner Mongolia Autonomous Region, China(No.2024KJTW0007), the Research Funds for Department of Education of Inner Mongolia Autonomous Region, China(No.NMGWDRW2025-05), the Innovative Research Team in Universities of Inner Mongolia Autonomous Region, China(No.NMGIRT2215), the Key Project of the Education Department of Inner Mongolia Autonomous Region, China(No.YLXKZX-NKD-003), the Inner Mongolia Autonomous Region Science and Technology Plan Project, China(Nos.2024SKYPT0035, 2025KYPT0164, 2025YFDZ0104), the “Young Scientific and Technological Talents Support Program” of Inner Mongolia Autonomous Region, China(No.NJYT24005)

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Abstract: To suppress the growth of lithium dendrites on lithium metal anodes，this study constructs a stable three-dimensional (3D) host structure of N-doped graphene/carbon nanotubes (N-G/CNTs) designed to suppress dendrite growth and facilitate long cycle life in lithium metal batteries. The N-G/CNTs composite was prepared via chemical vapor deposition (CVD) and pyrolysis, and subsequently mechanically calendered onto a lithium foil to obtain the N-G/CNTs-Li anode. Morphological characterization reveals that slender, curved CNTs are in-situ grafted onto the graphene substrate. First-principles calculations indicate that lithium preferentially nucleates and deposits on pyrrolic and pyridinic nitrogen sites. The N-G/CNTs half-cell exhibits a low nucleation overpotential of merely 21.3 mV. Furthermore, the N-G/CNTs-Li symmetric cell demonstrates stable cycling for up to 1000 h at a current density of 1 mA cm?2, maintaining minimal voltage polarization throughout. Post-cycling morphology after 100 hours shows a smooth and compact electrode surface, completely free of lithium dendrites. The full cell delivers a high capacity of 129.3 mAh g?1 and a capacity retention of 91.5% at a 1 C rate. These results collectively demonstrate that the N-G/CNTs host effectively mitigates electrode volume fluctuations and suppresses lithium dendrite growth during cycling. The excellent performance of the N-G/CNTs is attributed to the synergistic effect of the stability of the G/CNTs three-dimensional framework structure and the high content of the lithiophilic nitrogen species. Consequently, the N-G/CNTs-Li electrode holds great promise for applications in high-performance lithium metal batteries.

Key words: Graphene, Carbon nanotubes, N doping, Lithium dendrites; Long cycle life, Lithium metal anodes

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