Abstract
Metallic molybdenum disulfide (MoS2), e.g., 1T phase, is touted as a highly promising material for energy storage that already displays a great capacitive performance. However, due to its tendency to aggregate and restack, it remains a formidable challenge to assemble a high-performance electrode without scrambling the intrinsic structure. Here, we report an electrohydrodynamic-assisted fabrication of 3D crumpled MoS2 (c-MoS2) and its formation of an additive-free stable ink for scalable inkjet printing. The 3D c-MoS2 powders exhibited a high concentration of metallic 1T phase and an ultrathin structure. The aggregation-resistant properties of the 3D crumpled particles endow the electrodes with open space for electrolyte ion transport. Importantly, we experimentally discovered and theoretically validated that 3D 1T c-MoS2 enables an extended electrochemical stable working potential range and enhanced capacitive performance in a bivalent magnesium-ion aqueous electrolyte. With reduced graphene oxide (rGO) as the positive electrode material, we inkjet-printed 96 rigid asymmetric micro-supercapacitors (AMSCs) on a 4-in. Si/SiO2 wafer and 100 flexible AMSCs on photo paper. These AMSCs exhibited a wide stable working voltage of 1.75 V and excellent capacitance retention of 96% over 20 000 cycles for a single device. Our work highlights the promise of 3D layered materials as well-dispersed functional materials for large-scale printed flexible energy storage devices.
Highlights
Metallic molybdenum disulfide (MoS2), e.g., 1T phase, is touted as a highly promising material for energy storage that already displays a great capacitive performance
As a promising transition-metal dichalcogenides (TMDs) for energy storage devices,24−26 1T metallic molybdenum disulfide (MoS2) has been investigated extensively due to its unique layered structure, good electrochemical performance, and the earth abundance of bulk MoS2 as a mineral.[27−29] Typically, the 1T phase exhibits significantly enhanced hydrophilicity and an electrical conductivity at least 5 orders of magnitude higher than that of 2H-MoS2, which result in an extreme high volumetric capacitance of ∼700 F cm−3 in an aqueous electrolyte.[24]
Three-dimensional 1T crumpled MoS2 (c-MoS2) powders were obtained through the electrospray of chemically exfoliated MoS2 flakes, which were synthesized by a modified Li-intercalation process.[30]
Summary
Metallic molybdenum disulfide (MoS2), e.g., 1T phase, is touted as a highly promising material for energy storage that already displays a great capacitive performance. Even mixed with conductive 1T MoS2 flakes, the 2H phase dominated 3D cMoS2 still displayed a specific capacitance of only 143.3 F g−1 at 1 mV s−1, which rapidly dropped to 31.9 F g−1 when increasing the scan rate to 100 mV s−1 (Supplementary Figure S7a).
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