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ACS Nano


Title:"Multiple alkynes react with ethylene to enhance carbon nanotube synthesis, suggesting a polymerization-like formation mechanism"
Author(s):Plata DL; Meshot ER; Reddy CM; Hart AJ; Gschwend PM;
Address:"Department of Marine Chemistry and Geochemistry, Woods Hole Oceanographic Institution, Woods Hole, Massachusetts 02543, USA. dplata@alum.mit.edu"
Journal Title:ACS Nano
Year:2010
Volume:20101104
Issue:12
Page Number:7185 - 7192
DOI: 10.1021/nn101842g
ISSN/ISBN:1936-086X (Electronic) 1936-0851 (Linking)
Abstract:"Thermal treatments of feedstock gases (e.g., C(2)H(4)/H(2)) used during carbon nanotube (CNT) synthesis result in the formation of a complex mixture of volatile organic compounds and polycyclic aromatic hydrocarbons. Some of these are likely important CNT precursors, while others are superfluous and possibly degrade product quality, form amorphous carbon, and/or contribute to growth termination. To simulate the effect of thermal treatment without this chemical complexity, we delivered trace amounts of individual hydrocarbons, along with ethylene and hydrogen, to a cold-wall atmospheric pressure reactor containing a locally heated metal catalyst (Fe on Al(2)O(3)). Using these compound-specific experiments, we demonstrate that many alkynes (e.g., acetylene, methyl acetylene, and vinyl acetylene) accelerate multiwalled CNT formation with this catalyst system. Furthermore, ethylene is required for enhanced CNT growth, suggesting that the alkyne and ethylene may react in concert at the metal catalyst. This presents a distinct CNT formation mechanism where the chemical precursors may be intact during C-C bond formation, such as in polymerization reactions, challenging the widely accepted hypothesis that precursors completely dissociate into C (or C(2)) units before 'precipitating' from the metal. Armed with these mechanistic insights, we were able to form high-purity CNTs rapidly with a 15-fold improvement in yield, a 50% reduction in energetic costs, and order of magnitude reduction in unwanted byproduct formation (e.g., toxic and smog-forming chemicals and greenhouse gases)"
Keywords:
Notes:"PubMed-not-MEDLINEPlata, Desiree L Meshot, Eric R Reddy, Christopher M Hart, A John Gschwend, Philip M eng Research Support, Non-U.S. Gov't Research Support, U.S. Gov't, Non-P.H.S. 2010/11/06 ACS Nano. 2010 Dec 28; 4(12):7185-92. doi: 10.1021/nn101842g. Epub 2010 Nov 4"

 
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