高等学校化学学报

高等学校化学学报

• 研究论文 • 上一篇    下一篇

原位构建稳定的氮掺杂石墨烯/碳纳米管三维宿主实现无枝晶和长寿命锂金属负极

佘苏辉1,2，辛国祥1,2，包金小1,2，孙广澍1,2，王海涛3，宋金玲1,2，王青春1,2，布林朝克1,2，张金辉4   

  1. 1. 内蒙古科技大学材料科学与工程学院, 内蒙古自治区先进陶瓷材料与器件重点实验室 2. 轻稀土资源绿色提取与高效利用教育部重点实验室(内蒙古科技大学) 3. 湖南科霸汽车动力电池有限责任公司北京分公司 4. 唐山学院新材料与化学工程学院
  • 收稿日期:2026-04-20 修回日期:2026-05-30 网络首发:2026-06-01 发布日期:2026-06-01
  • 通讯作者: 辛国祥 E-mail:xinguoxiang@imust.edu.cn
  • 基金资助:
    国家自然科学基金(批准号：52362035, 22462023)、内蒙古自治区直属高校基本科研业务费项目(批准号：2023QNJS018)、内蒙古自治区科技突围项目(批准号：2024KJTW0007)、内蒙古自治区教育厅科研基金(批准号：NMGWDRW2025-05)、内蒙古自治区高校创新科研团队项目(批准号：NMGIRT2215)、内蒙古自治区教育厅重点项目(批准号：YLXKZX-NKD-003)、内蒙古自治区科技计划项目(批准号：2024SKYPT0035，2025KYPT0164, 2025YFDZ0104)和内蒙古自治区“青年科技人才支持计划”项目(批准号：NJYT24005)资助

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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摘要： 为了解决锂金属负极锂枝晶生长的问题，本研究构建了一种稳定的N掺杂石墨烯/碳纳米管(N-G/CNTs)三维宿主结构，它能够抑制枝晶生长，促进锂金属电池的长循环寿命。研究采用化学气相沉积和热解法制备N-G/CNTs，再经机械辊压到Li片获得N-G/CNTs-Li。N-G/CNTs形貌图可看出细长弯曲的CNTs原位接枝于石墨烯基体。根据第一性原理，锂更倾向于在吡咯N和吡啶N上形核沉积。N-G/CNTs半电池展示出仅为21.3 mV的形核过电位。N-G/CNTs-Li对称电池在1 mA cm-2下能稳定循环高达1000 h，在循环过程中始终保持最小的电压极化，循环100 h后极片呈现光滑紧密的形貌，无明显锂枝晶形成。全电池在1 C下展现出129.3 mAh g-1的容量和91.5%的容量保持率。结果表明，N-G/CNTs能够缓解循环过程中电极的体积变化，有效抑制锂枝晶生长。N-G/CNTs良好的性能归因于G/CNTs三维框架结构稳定性和高含量氮亲锂物种的协同效应。因此，N-G/CNTs-Li电极在锂金属电池中具有广阔的应用前景。

关键词: 石墨烯, 碳纳米管, 氮掺杂, 锂枝晶, 长循环寿命, 锂金属负极

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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