期刊
NANOSCALE
卷 4, 期 5, 页码 1695-1700出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c2nr11826b
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资金
- Marie Curie Fellowship from the Fundacao para a Ciencia e a Tecnologia, Portugal
- Marie Curie Action Cofund
- United States Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering
- Director, Office of Science, Office of Basic Energy Sciences
- U.S. Department of Energy [DE-AC02-05CH11231]
- Sandia National Laboratories
- U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]
Crystalline solids self-assembled from anionic and cationic porphyrins provide a new class of multifunctional optoelectronic micro- and nanomaterials. A 1 : 1 combination of zinc(II) tetra(4-sulfonatophenyl)porphyrin (ZnTPPS) and tin(IV) tetra(N-methyl-4-pyridiniumyl)porphyrin (SnTNMePyP) gives porphyrin nanosheets with high aspect ratios and varying thickness. The room temperature preparation of the nanosheets has provided the first X-ray crystal structure of a cooperative binary ionic (CBI) solid. The unit cell contains one and one-half molecules of aquo-ZnTPPS4- (an electron donor) and three half molecules of dihydroxy-SnTNMePyP4+ (an electron acceptor). Charge balance in the solid is reached without any non-porphyrinic ions, as previously determined for other CBI nanomaterials by non-crystallographic means. The crystal structure reveals a complicated molecular arrangement with slipped pi-pi stacking only occurring in isolated dimers of one of the symmetrically unique zinc porphyrins. Consistent with the crystal structure, UV-visible J-aggregate bands indicative of exciton delocalization and extended pi-pi stacking are not observed. XRD measurements show that the structure of the Zn/Sn nanosheets is distinct from that of Zn/Sn four-leaf clover-like CBI solids reported previously. In contrast with the Zn/Sn clovers that do exhibit J-aggregate bands and are photoconductive, the nanosheets are not photoconductive. Even so, the nanosheets act as light-harvesting structures in an artificial photosynthesis system capable of reducing water to hydrogen but not as efficiently as the Zn/Sn clovers.
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