水热法制备石墨烯的原子结构演变

董金帆,冯柳,杨玉莹,张强,王晶,范慧清,温广武,秦禄昌*

水热法制备石墨烯的原子结构演变

董金帆,冯柳,杨玉莹,张强,王晶,范慧清,温广武,秦禄昌*

(1.山东理工大学1.化学化工学院,2.分析测试中心,3.材料科学与工程学院,山东淄博255000;4.北卡大学物理与天文系,美国北卡教堂山 27599-3255)

     本研究通过球差校正透射电镜成像研究了氧化石墨烯还原到石墨烯的微观结构演变,并结合X射线光电子能谱和傅里叶红外光谱表征验证了还原过程含氧官能团的去除效果。氧化石墨烯的高分辨图像结构高度不均匀,氧化过程引入的氧原子与碳原子结合,破坏了C-C键结构形成sp3杂化键,使单层氧化石墨烯部分呈无序结构。还原后石墨烯可以清晰看到大范围的蜂窝状单晶结构,表明水热还原方法去除了大量含氧官能团,恢复了大部分共轭π键和碳原子sp2杂化结构,还原效果明显,碳氧比高达11.7。

关键词   氧化石墨烯;石墨烯;水热还原;原子结构

中图分类号:TB383;TG115. 21+5.3;Q246   文献标识码:A   doi:10.3969/j.issn.1000-6281.2024.02.007

 

Atomic structure evolution of graphene prepared by hydrothermal method

DONG Jinfan 1,FENGLiu 2,YANG Yuying 1, ZHANG Qiang 1, WANG Jin 1, FAN Huiqing 1,WEN Guangwu 3, QIN Luchang 4*

(1. School of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo Shandong 255000, China; 2. Analytical Testing Center, Shandong University of Technology, Zibo Shandong 255000, China; 3. School of Materials Science and Engineering, Shandong University of Technology, Zibo Shandong 255000, China; 4. Department of Physics and Astronomy, University of North Carolina at Chapel Hill, NC 27599-3255, USA)

Abstract   In this study, the microstructural evolution of reduced graphene oxide to graphene was investigated by spherical aberration-corrected TEM. The removal effect of oxygen-contained functional groups during the reduction process was verified by XPS and FTIR. The high-resolution structure of graphene oxide was highly inhomogeneous. The contrast between graphitic regions and disordered regions was obvious. Oxygen atoms introduced by oxidation process combined with carbon atoms and destroyed C-C bond structures to form sp3 hybridized bonds, making monolayer graphene oxide partly disordered. The C/O ratio in graphene oxide is 1.74. The C/O ratio in hydrothermally reduced graphene is increased to 11.71, proving that the reduction process removed many oxygenic functional groups. At a low magnification, graphene showed a light and thin lamella with large lateral dimensions and different degrees of surface folds. Spherical aberration-corrected TEM image showed that graphene had a nearly perfect honeycomb structure at atomic scale with few defects presented in the reduced graphene sample. The deoxygenation process restored most π-conjugated bonds and sp2 hybrid structure of carbon atoms, and the reduction effect was obvious. This study further demonstrated that spherical aberration-corrected transmission electron microscopy was an important method for material characterization. The combination of diffraction and imaging mode can broaden the atomic structure analysis of nanomaterials.

Keywords    graphene oxide; graphene; hydrothermal reduction; atomic structure

 

“全文下载请到同方知网,万方数据库或重庆维普等数据库中下载!”