The fabrication of three-dimensional (3D) graphene-based macroscopic materials with superior mechanical and electrical properties for flexible energy storage devices is still extremely challenging. Here, we report a novel 3D graphene hydrogel decorated by the biomass phytic acid (PAGH) with developed porosity and strengthen mechanical property via hydrothermal and freeze-drying methods. The phytic acid molecules are intercalated into the graphene sheets, enabling robust network structure. This induces the formation of materials with larger specific surface area, lower density and enhanced compressive strength compared with pure GH. When directly employed as an electrode, the PAGH exhibits a high specific capacitance of 248.8 F g⁻¹ at 1 A g⁻¹ and excellent rate performance of 67.9% as current density increasing to 20 A g⁻¹. Furthermore, the all-solid-state supercapacitor based PAGH can deliver outstanding cycle life (86.2% after cycling 10,000 times), glorious energy density (26.5 Wh kg⁻¹) and power density (5135.1 W kg⁻¹). The prepared device shows stable electrochemical behaviors at random bending angles. Therefore, the present work will open a new avenue to design and fabricate new flexible and portable graphene-based electrodes for future applications in energy storage devices.

具有用于柔性能量存储装置的具有优异的机械和电性能的三维（3D）石墨烯基宏观材料的制造仍然极具挑战性。在这里，我们报告了一种新型的3D石墨烯水凝胶，其由生物质植酸（PAGH）装饰而成，具有发达的孔隙率，并通过水热和冷冻干燥方法增强了机械性能。植酸分子插入石墨烯片中，从而实现稳健的网络结构。与纯GH相比，这导致形成具有更大的比表面积，更低的密度和增强的抗压强度的材料。当直接用作电极时，PAGH在1 A g ^-1时显示出248.8 F g ^-1的高比电容随着电流密度增加至20 A g ^-1，其优良的速率性能达到67.9％。此外，基于全固态超级电容器的PAGH可以提供出色的循环寿命（10,000次循环后为86.2％），光辉的能量密度（26.5 Wh kg ^-1）和功率密度（5135.1 W kg ^-1）。所制备的装置在随机弯曲角度下显示出稳定的电化学行为。因此，当前的工作将为设计和制造新的基于柔性和便携式石墨烯的电极开辟一条新途径，以供将来在储能设备中使用。