Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 2, Pages 467-471Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201809989
Keywords
black phosphorus; degradation mechanism; density functional calculations; hydroxide ion; nanostructures
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Funding
- National Key Research and Development Program of China [2016YFD0800305]
- National Natural Science Foundation of China [21607165, 41703107, 41603120]
- Open Foundation of State Key Laboratory of Environmental Criteria and Risk Assessment
- Chinese Research Academy of Environmental Sciences (sklecra OFP 2016)
- Youth Innovation Promotion Association CAS
- CAS Pioneer Hundred Talents Program
- Hundreds Talents Program of CAS
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The practical application of layered black phosphorus (LBP) is compromised by fast decomposition in the presence of H2O and/or O-2. The role of H2O is controversial. Herein, we propose a hydroxide ion (OH-)-initiated degradation mechanism for LBP to elucidate the role of H2O. We found that LBP degraded faster in alkaline solutions than in neutral or acidic solutions with or without O-2. Degradation rates of LBP increased linearly from pH 4 to 10. Density functional theory (DFT) calculations showed that OH- initiated the decomposition of LBP through breaking the P-P bond and forming a P-O bond. The detection of hypophosphite, generated from OH- reacting with P atoms, confirmed the hypothesis. Protons acted in a way distinctive from OH-, by inducing deposition/aggregation or forming a cation-pi layer to protect LBP from degradation. This work reveals the degradation mechanism of LBP and thus facilitates the development of effective stabilization technologies.
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