The piezo-response of two-dimensional molybdenum disulfide(MoS2) only exists at the edge of odd-number layers. It’s crucial to design reasonable micro/nano-structures and construct tight interfaces to weaken layer-dependence, enhance energy harvesting, charge transfer and active sites exposure to improve piezoelectricity. The novel sailboat-like-vertical-MoS2-nanosheets(SVMS), in which abundant vertical MoS2 nanosheets(∼20 nm, 1–5 layers) are uniformly distributed on horizontal substrate of MoS2, with abundant vertical interfaces and controllable phase composition are prepared by facile method. The larger geometric-asymmetry enhances mechanical energy capture. Experiment and theory revealed the enhanced in-/out-of-plane polarization, higher piezo-response in multi-directions and abundant active edge sites of SVMS, thereby eliminating the layer-dependence and generating higher piezo-potential. Cooperating with the Mo-S bonds at vertical interfaces, free electrons-holes are efficiently separated and migrated. The piezo-degradation of Rhodamine B(RhB) and hydrogen evolution rate under ultrasonic/stirring are 0.16 min−1 and 1598 μmolg−1h−1 for SVMS(2H) with the highest piezo-response (under ultrasonic wave, stirring and water flow), which are over 1.6 and 3.1 times than few-layer MoS2 nanosheets. 94% RhB(500 mL) is degraded under water-flow(60 min). The mechanism was proposed. Overall, the design of SVMS with enhanced piezoelectricity was studied and modulated by regulating microstructure and phase composition, which has excellent application potential in fields of environment, energy and novel materials.
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