Abstract:

The preparation of graphene by chemical vapor deposition (CVD) is a complex heterogeneous catalytic reaction process. It is of great significance to elucidate the scientific blueprint depicting this process in the viewpoint of catalysis engineering for deliberately structural control, standardization and application of graphene-based materials. Emphasizing on the recent research advance theoretically and experimentally, this review demonstrates how carbon precursors, reactive gases, catalytic metal substrates and carbon impurities are involved in the process, and reactive carbon-containing intermediates influence the graphene growth dynamics, as well as the macro- and micro- structural attributes (e.g., layer number, quality, shape, domain structure, etc.) of as-synthesized graphene. The motivation is to figure out the regulation principles for controllable preparation of graphene through excavating general scientific laws beneath the differentiated conclusions all over the research community. Additionally, several enhanced CVD approaches are introduced briefly, and essential roles of elementary reaction steps and reactive carbon-containing intermediates played in the controllable graphene synthesis are emphatically proposed. The knowledge is firmly contributable to define the controllable preparation of large-area graphene and its derived structure appealing to defect-free, super-clean, low-price, high-speed, and mass-scale advances.

Key words: graphene synthesis, heterogeneous reaction, thermodynamics, kinetics, reaction mechanism, structure control

摘要：

石墨烯的化学气相沉积(CVD)法制备是一个复杂的多相催化反应过程。如何从催化反应角度理解此过程中的诸多科学问题对石墨烯的精准结构控制以及石墨烯产品的标准化和实用化至关重要。结合最新研究进展，系统分析了CVD反应体系所包含的碳源、反应气氛、催化金属及其内部碳杂质、反应中间碳物种对石墨烯生长的热、动力学以及石墨烯宏、微观结构特性(层数、质量、形状、晶畴等)的影响机制和调控策略，挖掘不同石墨烯CVD反应体系背后的共性科学规律。简介了增强型CVD技术的发展，展望和建议基元反应步骤和含碳反应中间物种对于石墨烯控制制备的重要作用，为未来无缺陷、超洁净、低成本、快速、宏量化的大面积石墨烯薄膜及特定石墨烯衍生结构的定制化制备提供参考。

关键词: 石墨烯合成, 多相反应, 热力学, 动力学, 反应机理, 结构控制