Photocatalytic Carbon Disulfide Production via Charge Transfer Quenching of Quantum Dots
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- 作者：Christopher M. Bernt ; Peter T. Burks ; Anthony W. DeMartino ; Agustin E. Pierri ; Elizabeth S. Levy ; David F. Zigler ; Peter C. Ford
- 刊名：Journal of the American Chemical Society
- 出版年：2014
- 出版时间：February 12, 2014
- 年：2014
- 卷：136
- 期：6
- 页码：2192-2195
- 全文大小：229K
- ISSN：1520-5126
文摘
Carbon disulfide, a potentially therapeutic small molecule, is generated via oxidative cleavage of 1,1-dithiooxalate (DTO) photosensitized by CdSe quantum dots (QDs). Irradiation of DTO鈥換D conjugates leads to 位irr independent photooxidation with a quantum yield of 4% in aerated pH 9 buffer solution that drops sharply in deaerated solution. Excess DTO is similarly decomposed, indicating labile exchange at the QD surfaces and a photocatalytic cycle. Analogous photoreaction occurs with the O-tert-butyl ester tBuDTO in nonaqueous media. We propose that oxidation is initiated by hole transfer from photoexcited QD to surface DTO and that these substrates are a promising class of photocleavable ligands for modifying QD surface coordination.