Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 135, Issue 46, Pages 17595-17601Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja409657y
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Funding
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- Canada Foundation for Innovation (CFI)
- Alberta Science and Research Investment Program (ASRIP)
- University of Alberta Department of Chemistry
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Surface functionalization of hydride-terminated silicon nanocrystals (SiNCs) with dodecene via thermal hydrosilylation has been reexamined. We observed the formation of dodecyl oligomers (n <= 4) during the reaction under an argon atmosphere at various predesigned temperatures (100-190 degrees C). In a comparative study, surface hydrosilylation and ligand oligomerization were found to be more pronounced under air (n <= 7) at the same temperatures. These observations strongly suggest that hydrogen abstraction by oxygen accelerates hydrosilylation and generates sufficient silyl radical as initiator to interact with unsaturated bonds, promote chain propagation, and generate ligand oligomers. We further propose that, to inhibit ligand oligomerization and obtain monolayer coverage on SiNC surfaces, it is feasible to apply comparatively low temperatures, inert atmosphere, and dilute ligand concentration during thermal hydrosilylation.
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