Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 135, Issue 23, Pages 8492-8495Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja4035945
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Funding
- Department of Energy Office of Science Graduate Fellowship Program (DOE SCGF) in part by the American Recovery and Reinvestment Act [DE-AC05-06OR23100]
- ARCS Foundation
- American Chemical Society [51178-ND3]
- U.S. National Science Foundation [CHE-1151726]
- University of Washington
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1151726] Funding Source: National Science Foundation
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Electron transfer (ET) reactions of colloidal 3-5 nm diameter ZnO nanocrystals (NCs) with molecular reagents are explored in aprotic solvents. Addition of an excess of the one electron reductant Cp*Co-2 (Cp* = pentamethylcyclopentadienyl) gives NCs that are reduced by up to 1-3 electrons per NC. Protons can be added stoichiometrically to the NCs by either a photoreduction/oxidation sequence or by addition of acid. The added protons facilitate the reduction of the ZnO NCs. In the presence of acid, NC reduction by Cp*Co-2 can be increased to over 15 electrons per NC. The weaker reductant Cp*Cr-2 transfers electrons only to ZnO NCs in the presence of protons. Cp*M-2(+) counterions are much less effective than protons at stabilizing reduced NCs. With excess Cp*Co-2 or Cp*Cr-2, the extent of reduction increases roughly linearly with the number of protons added. Some of the challenges in understanding these results are discussed.
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