Journal
CHEM
Volume 6, Issue 1, Pages 221-233Publisher
CELL PRESS
DOI: 10.1016/j.chempr.2019.10.021
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Funding
- Natural Science Fund of China [11704365, GG2060190212, 21471142, 21671183, 21671181]
- National Key Research and Development Program of China [2017YFA0206703, 2016YFB0901500]
- National Postdoctoral Program for Innovative Talents [BX201700221]
- China Postdoctoral Science Foundation [2018M632546]
- Anhui Provincial Natural Science Foundation [1808085QB35, 1808085MB39]
- Fundamental Research Funds for the Central Universities [WK2060190074, WK2060190081, WK2060190053]
- USTC
- Recruitment Program of Global Experts
- National Synchrotron Radiation Laboratory (UN2018LHJJ)
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Evaporation-condensation of red phosphorous to prepare phosphorous-based anodes inevitably generates white P residual, severely limiting its practical application due to the serious safety concern. Rather than removing the white P residual by complicated post-treatments, essentially prohibiting the generation of white P is a more meaningful alternative, but unfortunately it has been rarely studied so far. Herein, we demonstrate that the generation of white P can be substantially suppressed via sulfur-mediated phosphorous activation. Moreover, the prepared sulfur-doped P also exhibits the ever-reported fastest redox kinetics for sodium-ion storage. Electron spin resonance spectra and density functional theory calculations reveal that the introduced sulfur lives in the high-spin state during the evaporation-condensation process, which could activate P-4 for polymerization. Meanwhile, sulfur-induced electron delocalization can also accelerate the Na-P redox kinetics. The capability to modulate phosphorus polymerization via the high-spin mediator could revolutionize the application of phosphorous for batteries and beyond.
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