Unveiling Surface Redox Charge Storage of Interacting Two-Dimensional Heteronanosheets in Hierarchical Architectures
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- Unveiling Surface Redox Charge Storage of Interacting Two-Dimensional Heteronanosheets in Hierarchical Architectures
- Mahmood, Qasim; Kim, Min Gyu; Yun, Sol; Bak, Seong-Min; Yang, Xiao-Qing; Shin, Hyeon Suk; Kim, Wook Sik; Braun, Paul V.; Park, Ho Seok
- Issue Date
- AMER CHEMICAL SOC
- NANO LETTERS, v.14, no.4, pp.2269 - 2277
- Two-dimensional (2D) heteronanosheets are currently the focus of intense study due to the unique properties that emerge from the interplay between two low-dimensional nanomaterials with different properties. However, the properties and new phenomena based on the two 2D heteronanosheets interacting in a 3D hierarchical architecture have yet to be explored. Here, we unveil the surface redox charge storage mechanism of surface-exposed WS2</inf> nanosheets assembled in a 3D hierarchical heterostructure using in situ synchrotron X-ray absorption and Raman spectroscopic methods. The surface dominating redox charge storage of WS2</inf> is manifested in a highly reversible and ultrafast capacitive fashion due to the interaction of heteronanosheets and the 3D connectivity of the hierarchical structure. In contrast, compositionally identical 2D WS2</inf> structures fail to provide a fast and high capacitance with different modes of lattice vibration. The distinctive surface capacitive behavior of 3D hierarchically structured heteronanosheets is associated with rapid proton accommodation into the in-plane W-S lattice (with the softening of the E2g</inf> bands), the reversible redox transition of the surface-exposed intralayers residing in the electrochemically active 1T phase of WS2</inf> (with the reversible change in the interatomic distance and peak intensity of W-W bonds), and the change in the oxidation state during the proton insertion/deinsertion process. This proposed mechanism agrees with the dramatic improvement in the capacitive performance of the two heteronanosheets coupled in the hierarchical structure.(Figure Presented). ⓒ 2015 American Chemical Society
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