Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 134, Issue 2, Pages 1085-1092Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja208878h
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Funding
- National Science Foundation [DMR-0906745]
- Department of Chemistry
- Dornsife College of Letters, Arts, and Science at University of Southern California
- Center for Energy Nanoscience, an Energy Frontier Research Center
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001013]
- Research Corporation for Science Advancement
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As-prepared CdSe nanocrystals were ligand exchanged using tert-butylthiol, which yielded stable CdSe nanocrystal inks in the strong donor solvent tetramethylurea. The efficacy of ligand exchange was probed by thermogravimetric analysis (TGA) and FT-IR spectroscopy. By studying sequential exchanges of tetradecylphosphonic acid and then tert-butylthiol, TGA and energy dispersive X-ray spectroscopic evidence clearly demonstrated that the ligand exchange is essentially quantitative. The resulting tert-butylthiol-exchanged CdSe nanocrystals undergo facile thermal ligand expulsion (<= 200 degrees C), which was studied by TGA-mass spectrometry. Mild thermal treatment of tert-butylthiol-exchanged CdSe nanocrystal films was found to induce loss of quantum confinement (as evidenced by UV-vis spectroscopy) and provided for increased electrochemical photocurrent, electron mobility, and film stability. Pyridine-exchanged CdSe nanocrystals were employed as a control system throughout to demonstrate the beneficial attributes of tert-butylthiol exchange; namely, lower organic content, better colloidal stability, improved interparticle coupling, and vastly increased electrochemical photocurrent response upon illumination.
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