In this work, the covalent attachment of an amine functionalized metal‐organic framework (UiO‐66‐NH₂ = Zr₆O₄(OH)₄(bdc‐NH₂)₆; bdc‐NH₂ = 2‐amino‐1,4‐benzenedicarboxylate) (UiO‐Universitetet i Oslo) to the basal‐plane of carboxylate functionalized graphene (graphene acid = GA) via amide bonds is reported. The resultant GA@UiO‐66‐NH₂ hybrid displayed a large specific surface area, hierarchical pores and an interconnected conductive network. The electrochemical characterizations demonstrated that the hybrid GA@UiO‐66‐NH₂ acts as an effective charge storing material with a capacitance of up to 651 F g⁻¹, significantly higher than traditional graphene‐based materials. The results suggest that the amide linkage plays a key role in the formation of a π‐conjugated structure, which facilitates charge transfer and consequently offers good capacitance and cycling stability. Furthermore, to realize the practical feasibility, an asymmetric supercapacitor using a GA@UiO‐66‐NH₂ positive electrode with Ti₃C₂T_X MXene as the opposing electrode has been constructed. The cell is able to deliver a power density of up to 16 kW kg⁻¹ and an energy density of up to 73 Wh kg⁻¹, which are comparable to several commercial devices such as Pb‐acid and Ni/MH batteries. Under an intermediate level of loading, the device retained 88% of its initial capacitance after 10 000 cycles.

中文翻译：

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高性能非对称超级电容器的共价石墨烯-MOF混合材料

在这项工作中，胺官能化的金属有机骨架（UiO-66-NH ₂  = Zr ₆ O ₄（OH）₄（bdc-NH ₂）₆； bdc-NH ₂  = 2-amino-1，据报道，4-氨基二羧酸盐（UiO-Universitetet i Oslo）通过酰胺键连接到羧酸盐官能化的石墨烯（石墨烯酸= GA）的基础平面上。生成的GA @ UiO-66-NH ₂杂化物显示出大的比表面积，分层的孔和相互连接的导电网络。电化学特性表明，杂化GA @ UiO-66-NH _2可作为有效的电荷存储材料，电容高达651 F g^-1，明显高于传统的基于石墨烯的材料。结果表明，酰胺键在π共轭结构的形成中起关键作用，它有助于电荷转移，因此具有良好的电容和循环稳定性。此外，为了实现实际可行性，已构建了一个非对称超级电容器，该超级电容器使用带有Ti ₃ C ₂ T _X MXene的GA @ UiO-66-NH ₂正极作为对电极。电池能够提供高达16 kW kg ^-1的功率密度和高达73 Wh kg ^-1的能量密度，可与多种商用设备（如铅酸电池和镍氢电池）媲美。在中等负载水平下，该器件在10000次循环后仍保持其初始电容的88％。