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Hybrid Nanocarbon as a Catalyst for Direct Dehydrogenation of Propane: Formation of an Active and Selective Core–Shell sp 2 /sp 3 Nanocomposite Structure
Author(s) -
Wang Rui,
Sun Xiaoyan,
Zhang Bingsen,
Sun Xiaoying,
Su Dangsheng
Publication year - 2014
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.201400018
Subject(s) - dehydrogenation , nanocomposite , nanodiamond , propane , catalysis , graphene , materials science , diamond , annealing (glass) , chemical engineering , propene , composite number , carbon fibers , nanotechnology , chemistry , composite material , organic chemistry , engineering
Hybrid nanocarbon, comprised of a diamond core and a graphitic shell with a variable sp 2 ‐/sp 3 ‐carbon ratio, is controllably obtained through sequential annealing treatment (550–1300 °C) of nanodiamond. The formation of sp 2 carbon increases with annealing temperature and the nanodiamond surface is reconstructed from amorphous into a well‐ordered, onion‐like carbon structure via an intermediate composite structure—a diamond core covered by a defective, curved graphene outer shell. Direct dehydrogenation of propane shows that the sp 2 ‐/sp 3 ‐nanocomposite exhibits superior catalytic performance to that of individual nanodiamond and graphitic nanocarbon. The optimum catalytic activity of the diamond/graphene composite depends on the maximum structural defectiveness and high chemical reactivity of the ketone groups. Ketone‐type functional groups anchored on the defects/vacancies are active for propene formation; nevertheless, once the oxygen functional groups are desorbed, the defects/vacancies alone might be active sites responsible for the CH bond activation of propane.