期刊
NATURE MATERIALS
卷 18, 期 2, 页码 156-+出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41563-018-0230-2
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资金
- R&D Convergence Program of the National Research Council of Science Technology [CAP-15-02-KBSI]
- National Research Foundation - Ministry of Science, ICT, and Future Planning [2017M2A2A6A01021187]
- Energy Technology Development Project (ETDP) - Ministry of Trade, Industry, and Energy, Republic of Korea [20172410100150]
- US Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) [70NANB14H012]
- Office of the Provost
- Northwestern University Information Technology
- Office for Research
- Korea Evaluation Institute of Industrial Technology (KEIT) [20172410100150] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
- National Research Foundation of Korea [2017M2A2A6A01021187] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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 similar to 72% (compared to 21.2% for black phosphorus) and retention of similar to 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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