期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 53, 期 21, 页码 5371-5375出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201402444
关键词
cyclophanes; electron transfer; ExBox; femtochemistry; photochemistry
资金
- Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, DOE [DE-FG02-99ER14999]
- Joint Center of Excellence in Integrated Nano-Systems (JCIN) at the King Abdulaziz City of Science and Technology (KACST) [34-947]
- Northwestern University (NU)
- Camille and Henry Dreyfus Postdoctoral Program in Environmental Chemistry
- ANSER Center, an Energy Frontier Research Center
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001059]
- Department of Defense [32 CFR 168a]
- Department of Energy
- NU International Institute for Nanotechnology (IIN)
- The Netherlands Organisation for Scientific Research (NWO)
- Marie Curie Cofund Action (Rubicon Fellowship)
Molecules capable of accepting and storing multiple electrons are crucial components of artificial photosynthetic systems designed to drive catalysts, such as those used to reduce protons to hydrogen. ExBox(4+), a boxlike cyclophane comprising two -electron-poor extended viologen units tethered at both ends by two p-xylylene linkers, has been shown previously to accept an electron through space from a photoexcited guest. Herein is an investigation of an alternate, through-bond intramolecular electron-transfer pathway involving ExBox(4+) using a combination of transient absorption and femtosecond stimulated Raman spectroscopy (FSRS). Upon photoexcitation of ExBox(4+), an electron is transferred from one of the p-xylylene linkers to one of the extended viologen units in ca. 240ps and recombines in ca. 4ns. A crystal structure of the doubly reduced species ExBox(2+) was obtained.
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