Eng Alex Yong Sheng, Chua Chun Kiang, Pumera Martin
Division of Chemistry & Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371, Singapore.
Phys Chem Chem Phys. 2016 Apr 14;18(14):9673-81. doi: 10.1039/c5cp07254a.
The majority of supercapacitor research studies on graphene materials today have been based upon developing electrochemical double-layer capacitors (EDLCs) using reduced graphenes. In contrast, graphene oxide (GO) is often neglected as a supercapacitor candidate due to its low electrical conductivity and surface area. Nonetheless, we present herein a fast (1 h) labelling of GO with o-phenylenediamine (PD) to produce PD-GO, exploiting inherent oxygen groups in creating new functionalities that exhibit capacitive enhancement from pseudo-capacitance. A high specific capacitance of 191 F g(-1) was obtained (at 0.2 A g(-1)), comparable to recent binder-free graphene supercapacitors. The large surface-normalized capacitance of up to 628 μF cm(-2) is also many times greater than the intrinsic capacitance of single-layer graphene (21 μF cm(-2)) as a result of additional pseudo-capacitance. A high capacity retention of ∼85% with each 10-fold increase in current density further indicates excellent rate performance. Hence, this approach in enhancing GO pseudo-capacitance may be similarly feasible as graphene EDLCs. Additionally, PD-GO was also found to exhibit a bright green fluorescence with a 540 nm maximum. The strongest fluorescence intensities arose from the smallest PD-GO fragments, and we attribute the origin to localised sp(2) domains and newly formed phenazine edge groups. The dual enhancement of dissimilar properties such as capacitance and fluorescence emphasizes the continued significance of covalent functionalisation towards tuning of properties in graphene-type materials.
如今,大多数关于石墨烯材料的超级电容器研究都是基于使用还原石墨烯开发电化学双层电容器(EDLC)。相比之下,氧化石墨烯(GO)由于其低电导率和表面积,常被忽视作为超级电容器候选材料。尽管如此,我们在此展示了一种用邻苯二胺(PD)对GO进行快速(1小时)标记以制备PD-GO的方法,利用其固有氧基团创造新功能,这些功能表现出赝电容导致的电容增强。在0.2 A g⁻¹时获得了191 F g⁻¹的高比电容,与最近的无粘合剂石墨烯超级电容器相当。由于额外的赝电容,高达628 μF cm⁻²的大表面归一化电容也比单层石墨烯的固有电容(21 μF cm⁻²)大许多倍。随着电流密度每增加10倍,容量保持率高达约85%,这进一步表明其优异的倍率性能。因此,这种增强GO赝电容的方法可能与石墨烯EDLC同样可行。此外,还发现PD-GO在540 nm处呈现亮绿色荧光。最强的荧光强度来自最小的PD-GO片段,我们将其归因于局域化的sp²域和新形成的吩嗪边缘基团。电容和荧光等不同性质的双重增强强调了共价功能化在调节石墨烯类材料性质方面的持续重要性。