One Step Formation of Propene from Ethene or Ethanol through Metathesis on Nickel Ion-loaded Silica 英文参考文献.docVIP

Molecules 2011, 16, 7844-7863; doi:10.3390/moleculeOPEN ACCESS molecules ISSN 1420-3049 /journal/molecules Review One Step Formation of Propene from Ethene or Ethanol through Metathesis on Nickel Ion-loaded Silica Masakazu Iwamoto Chemical Resources Laboratory, Tokyo Institute of Technology, 4259-R1-5 Nagatsuta, Midori-ku, Yokohama 226-8503, Japan; E-Mail: iwamoto@res.titech.ac.jp; Tel.: +81-45-924-5225; Fax: +81-45-924-5228 Received: 30 June 2011; in revised form: 4 August 2011 / Accepted: 5 September 2011 / Published: 13 September 2011 Abstract: Increased propene production is presently one of the most significant objectives in petroleum chemistry. Especially the one-step conversion of ethene to propene (ETP reaction, 3C2H4 → 2C3H6) is the most desired process. In our efforts, nickel ion-loaded mesoporous silica could turn a new type of ETP reaction into reality. The one-step conversion of ethene was 68% and the propene selectivity was 48% in a continuous gas-flow system at 673 K and atmospheric pressure. The reactivity of lower olefins and the dependences of the ETP reaction on the contact time and the partial pressure of ethene were consistent with a reaction mechanism involving dimerization of ethene to 1-butene, isomerization of 1-butene to 2-butene, and metathesis of 2-butene and ethene to yield propene. The reaction was then expanded to an ethanol-to-propene reaction on the same catalyst, in which two possible reaction routes are suggested to form ethene from ethanol. The catalysts were characterized mainly by EXAFS and TPR techniques. The local structures of the nickel species active for the ETP reaction were very similar to that of layered nickel silicate, while those on the inert catalysts were the same as that of NiO particles. Keywords: ethene; ethanol; propene; metathesis; nickel; mesoporous silica 1. Introduction The mainsta