TY - JOUR
T1 - Synergy between Two Metal Catalysts: A Highly Active Silica Supported Bimetallic W/Zr Catalyst for Metathesis of n-Decane
AU - Samantaray, Manoja
AU - Dey, Raju
AU - Kavitake, Santosh Giridhar
AU - Abou-Hamad, Edy
AU - Bendjeriou-Sedjerari, Anissa
AU - Hamieh, Ali Imad Ali
AU - Basset, Jean-Marie
N1 - KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: The authors acknowledge the KAUST Nuclear Magnetic Resonance
Core Lab and analytical core lab (ACL) for the analysis
of the sample. This publication is based upon work supported
by the King Abdullah University of Science and Technology
(KAUST) Office of Sponsored Research (OSR).
PY - 2016/6/28
Y1 - 2016/6/28
N2 - A well-defined, silica supported, bimetallic precatalyst [≡Si-O-W(Me)5 ≡Si-O-Zr(Np)3](4) has been synthesized for the first time via successively grafting two organometallic complexes [W(CH3)6 (1) followed by ZrNp4 (2)] on a single silica support. Surprisingly, multiple quantum NMR characterization demonstrates that W and Zr species are in close proximity to each other. Hydrogenation of this bimetallic catalyst at room temperature showed the easy formation of Zirconium hydride, probably facilitated by tungsten hydride which was formed at this temperature. This bimetallic W/Zr hydride precatalyst proved to be more efficient (TON: 1436) than the monometallic W hydride (TON: 650) in metathesis of n-decane at 150 0C. This synergy between Zr and W suggests that the slow step of alkane metathesis is the C-H bond activation which occurs on Zr. The produced olefin resulting from a ß–H elimination undergoes easy metathesis on W.
AB - A well-defined, silica supported, bimetallic precatalyst [≡Si-O-W(Me)5 ≡Si-O-Zr(Np)3](4) has been synthesized for the first time via successively grafting two organometallic complexes [W(CH3)6 (1) followed by ZrNp4 (2)] on a single silica support. Surprisingly, multiple quantum NMR characterization demonstrates that W and Zr species are in close proximity to each other. Hydrogenation of this bimetallic catalyst at room temperature showed the easy formation of Zirconium hydride, probably facilitated by tungsten hydride which was formed at this temperature. This bimetallic W/Zr hydride precatalyst proved to be more efficient (TON: 1436) than the monometallic W hydride (TON: 650) in metathesis of n-decane at 150 0C. This synergy between Zr and W suggests that the slow step of alkane metathesis is the C-H bond activation which occurs on Zr. The produced olefin resulting from a ß–H elimination undergoes easy metathesis on W.
UR - http://hdl.handle.net/10754/613000
UR - http://pubs.acs.org/doi/abs/10.1021/jacs.6b04307
UR - http://www.scopus.com/inward/record.url?scp=84978807238&partnerID=8YFLogxK
U2 - 10.1021/jacs.6b04307
DO - 10.1021/jacs.6b04307
M3 - Article
C2 - 27248839
SN - 0002-7863
VL - 138
SP - 8595
EP - 8602
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 27
ER -