Revealing molecular-level surface redox sites of controllably oxidized black phosphorus nanosheets
- Revealing molecular-level surface redox sites of controllably oxidized black phosphorus nanosheets
- 황준연; 이원기; Puritu Nakhanivej; Xu Yu; 박슬기; 김수; 홍진용; 김해진; 양지윤; Chris Wolverton; Jing Kong; Manish Chhowalla; 박호석
- Black phosphorus
- Issue Date
- Nature materials
- VOL 18-162
- Bulk and two-dimensional black phosphorus are considered to be promising battery materials due to their high theoretical capacities of 2,600  mAh g− 1. However, their rate and cycling capabilities are limited by the intrinsic (de-)alloying mechanism. Here, we demonstrate a unique surface redox molecular-level mechanism of P sites on oxidized black phosphorus nanosheets that are strongly coupled with graphene via strong interlayer bonding. These redox-active sites of the oxidized black phosphorus are confined at the amorphorized heterointerface, revealing truly reversible pseudocapacitance (99% of total stored charge at 2,000  mV  s− 1). Moreover, oxidized black-phosphorus-based electrodes exhibit a capacitance of 478  F  g– 1 (four times greater than black phosphorus) with a rate capability of ~72% (compared to 21.2% for black phosphorus) and retention of ~91% over 50,000 cycles. In situ spectroelectrochemical and theoretical analyses reveal a reversible change in the surface electronic structure and chemical environment of the surface-exposed P redox sites.
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