Journal
NATURE CHEMISTRY
Volume 9, Issue 7, Pages 644-652Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.2765
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Funding
- UK Engineering and Physical Sciences Research Council [EP/K027255, EP/K027212]
- European Union/JST SICORP-LEMSUPER FP7-NMP-EU-Japan project [NMP3-SL-2011-283214]
- Mitsubishi Foundation
- Japan Society for the Promotion of Science [15H05882]
- World Premier International (WPI) Research Center Initiative for Atoms, Molecules and Materials
- Ministry of Education, Culture, Sports, Science, and Technology of Japan
- Japan Science and Technology Agency under the ERATO Isobe Degenerate p-Integration Project
- Royal Society
- Grants-in-Aid for Scientific Research [16H01063] Funding Source: KAKEN
- Engineering and Physical Sciences Research Council [EP/K027255/2, EP/K027212/1] Funding Source: researchfish
- EPSRC [EP/K027212/1, EP/K027255/2] Funding Source: UKRI
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Alkali metal intercalation into polyaromatic hydrocarbons (PAHs) has been studied intensely after reports of superconductivity in a number of potassium-and rubidium-intercalated materials. There are, however, no reported crystal structures to inform our understanding of the chemistry and physics because of the complex reactivity of PAHs with strong reducing agents at high temperature. Here we present the synthesis of crystalline K(2)Pentacene and K(2)Picene by a solid-solid insertion protocol that uses potassium hydride as a redox-controlled reducing agent to access the PAH dianions, and so enables the determination of their crystal structures. In both cases, the inserted cations expand the parent herringbone packings by reorienting the molecular anions to create multiple potassium sites within initially dense molecular layers, and thus interact with the PAH anion pi systems. The synthetic and crystal chemistry of alkali metal intercalation into PAHs differs from that into fullerenes and graphite, in which the cation sites are pre-defined by the host structure.
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