Journal
SCIENCE
Volume 329, Issue 5997, Pages 1324-1327Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1192044
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Funding
- Ministry of Education, Culture, Sports, Science and Technology, Japan
- NSF [CHE 0749571, 0741973]
- R.A. Welch Foundation [F-1018, E-680, F-1621]
- Korean World Class University [R32-20080-000-10217-0, R31-2008-000-10010-0]
- [20108010]
- Grants-in-Aid for Scientific Research [20108001] Funding Source: KAKEN
- Ministry of Education, Science & Technology (MoST), Republic of Korea [R32-2008-000-10217-0] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
- National Research Foundation of Korea [R31-2008-000-10010-0] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [741973] Funding Source: National Science Foundation
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Ion binding often mediates electron transfer in biological systems as a cofactor strategy, either as a promoter or as an inhibitor. However, it has rarely, if ever, been exploited for that purpose in synthetic host-guest assemblies. We report here that strong binding of specific anions (chloride, bromide, and methylsulfate but not tetrafluoroborate or hexafluorophosphate) to a tetrathiafulvalene calix[4]pyrrole (TTF-C4P) donor enforces a host conformation that favors electron transfer to a bisimidazolium quinone (BIQ(2+)) guest acceptor. In contrast, the addition of a tetraethylammonium cation, which binds more effectively than the BIQ(2+) guest in the TTF-C4P cavity, leads to back electron transfer, restoring the initial oxidation states of the donor and acceptor pair. The products of these processes were characterized via spectroscopy and x-ray crystallography.
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