A new mechanism of catalyst has been demonstrated in this article. With the interaction between carbon nitride(CN) and encapsulated nickel, the CN in the catalyst has been endowed with new active sites for the adsorpt...A new mechanism of catalyst has been demonstrated in this article. With the interaction between carbon nitride(CN) and encapsulated nickel, the CN in the catalyst has been endowed with new active sites for the adsorption and activation of hydrogen while nickel itself is physically isolated from the contact with reactive molecules. For the selective hydrogenation of acetylene in large amount of ethylene, the catalyst shows excellent ethylene selectivity than the nickel catalyst itself, which is almost totally unselective. Meanwhile, the CN itself is inactive for the reaction. The results of characterization demonstrate that pyridinic nitrogen doped in the carbon matrix should be the active sites for hydrogen dissociative adsorption. The theoretical calculations further confirm the results and provide with the detail in the electron transfer between nickel and CN in the catalyst. The current results supply a new concept for design of high performance catalyst.展开更多
基金supported by the Science Foundation of Hebei Province(B2012402001,D2014402046)Program for One Hundred Innovative Talents in Universities of Hebei Province(BR2-204)and the Science and Technology Foundation of Universities of Hebei Province(Q2012030)~~
文摘A new mechanism of catalyst has been demonstrated in this article. With the interaction between carbon nitride(CN) and encapsulated nickel, the CN in the catalyst has been endowed with new active sites for the adsorption and activation of hydrogen while nickel itself is physically isolated from the contact with reactive molecules. For the selective hydrogenation of acetylene in large amount of ethylene, the catalyst shows excellent ethylene selectivity than the nickel catalyst itself, which is almost totally unselective. Meanwhile, the CN itself is inactive for the reaction. The results of characterization demonstrate that pyridinic nitrogen doped in the carbon matrix should be the active sites for hydrogen dissociative adsorption. The theoretical calculations further confirm the results and provide with the detail in the electron transfer between nickel and CN in the catalyst. The current results supply a new concept for design of high performance catalyst.
