Phthalocyanine-based 2D conjugated metal-organic framework nanosheets for high-performance micro-supercapacitors

2D conjugated metal-organic frameworks (2D c-MOFs) are emerging as a novel class of conductive redox-active materials for electrochemical energy storage. However, developing 2D c-MOFs as flexible thin-film electrodes have been largely limited, due to the lack of capability of solution-processing and integration into nanodevices arising from the rigid powder samples by solvothermal synthesis. Here, the synthesis of phthalocyanine-based 2D c-MOF (Ni2[CuPc(NH)8]) nanosheets through ball milling mechanical exfoliation method are reported. The nanosheets feature with average lateral size of ≈160 nm and mean thickness of ≈7 nm (≈10 layers), and exhibit high crystallinity and chemical stability as well as a p-type semiconducting behavior with mobility of ≈1.5 cm2 V−1 s−1 at room temperature. Benefiting from the ultrathin feature, the nanosheets allow high utilization of active sites and facile solution-processability. Thus, micro-supercapacitor (MSC) devices are fabricated mixing Ni2[CuPc(NH)8] nanosheets with exfoliated graphene, which display outstanding cycling stability and a high areal capacitance up to 18.9 mF cm−2; the performance surpasses most of the reported conducting polymers-based and 2D materials-based MSCs.