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dc.contributor.authorIritani, Koheien_US
dc.contributor.authorTakeda, Hiroshien_US
dc.contributor.authorKather, Michaelen_US
dc.contributor.authorYokoi, Masahikoen_US
dc.contributor.authorMoeglen, Magalien_US
dc.contributor.authorIkeda, Motokien_US
dc.contributor.authorOtsubo, Yusukeen_US
dc.contributor.authorOzawa, Yuen_US
dc.contributor.authorTahara, Kazukunien_US
dc.contributor.authorHirose, Keijien_US
dc.contributor.authorDe Feyter, Stevenen_US
dc.contributor.authorTobe, Yoshitoen_US
dc.date.accessioned2020-01-02T00:04:24Z-
dc.date.available2020-01-02T00:04:24Z-
dc.date.issued2019-11-26en_US
dc.identifier.issn0743-7463en_US
dc.identifier.urihttp://dx.doi.org/10.1021/acs.langmuir.9b02748en_US
dc.identifier.urihttp://hdl.handle.net/11536/153441-
dc.description.abstractWe present here the construction of a self-assembled two-dimensional network at the liquid/solid interface using a hexagonal pyridine macrocycle which binds an organic cation in its intrinsic porous space by electrostatic interactions. For this purpose, a hexagonal pyridinylene-butadiynylene macrocycle (PyBM) having six octyloxymethyl groups, PyBM-C8, was synthesized. As guests, tropylium (Tr) tetrafluoroborate and trioxatriangulenium (TOTA) hexafluorophosphate were used. In this study, we focused on (i) the network patterns of PyBM-C8 which change in response to its concentration and (ii) the position of the guest immobilized in the porous space of the macrocycle. Scanning tunneling microscopy (STM) observations at the interface of 1,2,4-trichlorobenzene (TCB) and highly oriented pyrolytic graphite (HOPG) revealed that PyBM-C8 formed four different polymorphs, oblique, loose hexagonal, linear, and rectangular, depending on the solute concentration and annealing treatment. Solvent TCB molecules are likely coadsorbed to not only the intrinsically porous space of PyBM-C8 (internal TCB) but also the space outside of the macrocycle between its alkyl chains (external TCB) in most of the cases. Upon adding the guest cation, whereas small Tr was not visualized in the pore due to size mismatching, larger TOTA was clearly observed in each pore. In addition, based on high-resolution STM images of the rhombus packing pattern of PyBM-C8, we revealed experimentally that TOTA was placed at an off center position of the deformed hexagonal macrocyclic core in the rhombus pattern. On the basis of the molecular mechanics calculations, we hypothesize that the off-center location of TOTA is due to deformation of the hexagonal macrocycle through interaction with two external TCB molecules located at opposite edges of the macrocyclic core. Symmetry breaking of the macrocyclic host framework induced by coadsorbed surrounding solvent molecules thus plays a significant role in host-guest complexation at the liquid/solid interface.en_US
dc.language.isoen_USen_US
dc.titleElectrostatically Driven Guest Binding in Self-Assembled Molecular Network of Hexagonal Pyridine Macrocycle at the Liquid/Solid Interface: Symmetry Breaking Induced by Coadsorbed Solvent Moleculesen_US
dc.typeArticleen_US
dc.identifier.doi10.1021/acs.langmuir.9b02748en_US
dc.identifier.journalLANGMUIRen_US
dc.citation.volume35en_US
dc.citation.issue47en_US
dc.citation.spage15051en_US
dc.citation.epage15062en_US
dc.contributor.department應用化學系zh_TW
dc.contributor.departmentDepartment of Applied Chemistryen_US
dc.identifier.wosnumberWOS:000500039900009en_US
dc.citation.woscount0en_US
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