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郁旭博士(共同一作)在Nature Materials上发表研究论文
发布日期:2019-06-03 浏览次数: 字号:[ ]

Revealing molecular-level surface redox sites of controllably oxidized black phosphorus nanosheets

 

Nakhanivej Puritut1,11, Yu Xu1,10,11, Park Sul Ki1, Kim Soo2,3, Hong Jin-Yong4,5, Kim Hae Jin6, Lee Wonki7, Hwang Jun Yeon7, Yang Ji Eun8, Wolverton Chris2, Kong Jing4, Chhowalla Manish8, Park Ho Seok1,9*

 

1School of Chemical Engineering, College of Engineering, Sungkyunkwan University, Suwon, Republic of Korea

10School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, China.

11These authors contributed equally: Puritut Nakhanivej, Xu Yu

 

Abstract: 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.

 

(a) Schematic model of the foBG film showing adsorption sites, charge storage and charge transfer mechanism; (b) Rate capability of 2D BP, rGO, oBGO and foBG at various current densities from 1 to 50 A g–1.

 

Nature Materials, 2019, 18, 156-162; Doi: 10.1038/s41563-018-0230-2. IF: 39.235

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