物理化学学报 >> 2022, Vol. 38 >> Issue (1): 2101053.doi: 10.3866/PKU.WHXB202101053

所属专题: 石墨烯的功能与应用

综述 上一篇    下一篇

气相反应对CVD生长石墨烯的影响

陈恒1,3, 张金灿1,2,3, 刘晓婷1,2,3, 刘忠范1,3,*()   

  1. 1 北京大学纳米化学研究中心,北京分子科学国家研究中心,北京大学化学与分子工程学院,北京 100871
    2 北京大学前沿交叉学科研究院,北京 100871
    3 北京石墨烯研究院,北京 100095
  • 收稿日期:2021-01-27 录用日期:2021-02-22 发布日期:2021-03-01
  • 通讯作者: 刘忠范 E-mail:zfliu@pku.edu.cn
  • 作者简介:刘忠范,1962年出生。1990年获东京大学博士学位。现为北京大学教授,博士生导师,北京石墨烯研究院院长,中国科学院院士。主要研究方向为石墨烯的CVD生长方法与应用第一联系人:

    These authors contributed equally to this work.

  • 基金资助:
    国家重点基础研究发展规划项目(2016YFA0200103);国家重点基础研究发展规划项目(2018YFA0703502);国家自然科学基金(51520105003);国家自然科学基金(52072042);北京分子科学国家研究中心(BNLMS-CXTD-202001);北京市科学技术委员会(Z18110300480001);北京市科学技术委员会(Z18110300480002)

Effect of Gas-Phase Reaction on the CVD Growth of Graphene

Heng Chen1,3, Jincan Zhang1,2,3, Xiaoting Liu1,2,3, Zhongfan Liu1,3,*()   

  1. 1 Center for Nanochemistry, Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China
    2 Academy for Advanced Interdisciplinary Studies, Peking University, Beijing 100871, China
    3 Beijing Graphene Institute (BGI), Beijing 100095, China
  • Received:2021-01-27 Accepted:2021-02-22 Published:2021-03-01
  • Contact: Zhongfan Liu E-mail:zfliu@pku.edu.cn
  • About author:Zhongfan Liu, Email: zfliu@pku.edu.cn
  • Supported by:
    the National Key Basic Research Program of China(2016YFA0200103);the National Key Basic Research Program of China(2018YFA0703502);the National Natural Science Foundation of China(51520105003);the National Natural Science Foundation of China(52072042);Beijing National Laboratory for Molecular Sciences(BNLMS-CXTD-202001);the Beijing Municipal Science and Technology Planning Project(Z18110300480001);the Beijing Municipal Science and Technology Planning Project(Z18110300480002)

摘要:

化学气相沉积法(CVD)制备的石墨烯薄膜具有质量高、均匀性好、层数可控且可放大等优点,近年来受到了学术界和工业界的广泛关注。在高温CVD生长过程中,除衬底表面的反应外,气相反应同样会影响石墨烯的生长行为和薄膜质量。本文将综述气相反应对CVD生长石墨烯的影响:首先对CVD体系内的气相传质过程和气相反应进行了详细讨论;随后系统介绍了基于气相调控提高石墨烯的结晶性、洁净度、畴区尺寸、层数和生长速度的相关策略及其机理;最后对气相反应影响CVD生长石墨烯的规律进行总结,并展望了未来可能的发展方向。

关键词: 石墨烯薄膜, 化学气相沉积, 气相反应, 高品质, 可控制备

Abstract:

Chemical vapor deposition (CVD) is considered as the most promising method for the mass production of high-quality graphene films owing to its fine controllability, uniformity, and scalability. In the past decade, significant efforts have been devoted to exploring new strategies for growing graphene with improved quality. During the high-temperature CVD growth process of graphene, besides the surface reactions, gas-phase reactions play an important role in the growth of graphene, especially for the decomposition of hydrocarbons. However, the effect of gas-phase reactions on the CVD growth of graphene has not been analyzed previously. To fill this gap, it is essential to systematically analyze the relationship between gas-phase reactions and the growth of graphene films. In this review article, we aim to provide comprehensive knowledge of the gas-phase reactions occurring in the CVD system during graphene growth and to summarize the typical strategies for improving the quality of graphene by modulating gas-phase reactions. After briefly introducing the elementary steps and basic concept of graphene growth, we focus on the gas-phase dynamics and reactions in the CVD system, which influence the decomposition of hydrocarbons, nucleation of graphene, and lateral growth of graphene nuclei, as well as the merging of adjacent graphene domains. Then, a systematic description of the mass transport process in gas phase is provided, including confirmation of the states of gas flow under different CVD conditions and introduction to the boundary layer, which is crucial for graphene growth. Furthermore, we discuss the possible reaction paths of carbon sources in the gas phase and the corresponding active carbon species existing in the boundary layer, based on which the main impact factors of gas-phase reactions are discussed. Representative strategies for obtaining graphene films with improved quality by modulating gas-phase reactions are summarized. Gas-phase reactions affect the crystallinity, cleanness, domain size, layer number, and growth rate of graphene grown on both metal and non-metal substrates. Therefore, we will separately review the detailed strategies, corresponding mechanisms, key parameters, and latest status regarding the quality improvement of graphene. Finally, a brief summary and proposals for future research are provided. This review can be divided into two parts: (1) gas-phase reactions occurring in the high-temperature CVD system, including the mass transport process and the reaction paths of hydrocarbons; and (2) the synthesis of high-quality graphene film via modulation of the gas-phase reaction, in order to improve the crystallinity, cleanness, domain size, layer number, and growth rate of graphene.

Key words: Graphene film, Chemical vapor deposition, Gas-phase reaction, High quality, Controlled synthesis

MSC2000: 

  • O647