Metallic
molybdenum disulfide (MoS
2
),
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 MoS
2
(c-MoS
2
) and
its formation of an additive-free stable ink for scalable inkjet printing.
The 3D c-MoS
2
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-MoS
2
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/SiO
2
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.