Imperial College London
Alternate

Dr Rob Davies

Faculty of Natural Sciences, Department of Chemistry

Reader in Inorganic Chemistry
 
 
 
//

Contact

 

+44 (0)20 7594 5754r.davies

 
 
//

Location

 

601JMolecular Sciences Research HubWhite City Campus

//

Summary

 

Publications

Citation

BibTex format

@article{Grigoropoulos:2016:10.1039/c5sc03494a,
author = {Grigoropoulos, A and Whitehead, GFS and Perret, N and Katsoulidis, AP and Chadwick, FM and Davies, RP and Haynes, A and Brammer, L and Weller, AS and Xiao, J and Rosseinsky, MJ},
doi = {10.1039/c5sc03494a},
journal = {Chemical Science},
pages = {2037--2050},
title = {Encapsulation of an organometallic cationic catalyst by direct exchange into an anionic MOF},
url = {http://dx.doi.org/10.1039/c5sc03494a},
volume = {7},
year = {2016}
}
Download

RIS format (EndNote, RefMan)

TY  - JOUR
AB  - Metal–Organic Frameworks (MOFs) are porous crystalline materials that have emerged as promising hosts for the heterogenization of homogeneous organometallic catalysts, forming hybrid materials which combine the benefits of both classes of catalysts. Herein, we report the encapsulation of the organometallic cationic Lewis acidic catalyst [CpFe(CO)2(L)]+ ([Fp–L]+, Cp = η5-C5H5, L = weakly bound solvent) inside the pores of the anionic [Et4N]3[In3(BTC)4] MOF (H3BTC = benzenetricarboxylic acid) via a direct one-step cation exchange process. To conclusively validate this methodology, initially [Cp2Co]+ was used as an inert spatial probe to (i) test the stability of the selected host; (ii) monitor the stoichiometry of the cation exchange process and (iii) assess pore dimensions, spatial location of the cationic species and guest-accessible space by single crystal X-ray crystallography. Subsequently, the quasi-isosteric [Fp–L]+ was encapsulated inside the pores via partial cation exchange to form [(Fp–L)0.6(Et4N)2.4][In3(BTC)4]. The latter was rigorously characterized and benchmarked as a heterogeneous catalyst in a simple Diels–Alder reaction, thus verifying the integrity and reactivity of the encapsulated molecular catalyst. These results provide a platform for the development of heterogeneous catalysts with chemically and spatially well-defined catalytic sites by direct exchange of cationic catalysts into anionic MOFs.
AU  - Grigoropoulos,A
AU  - Whitehead,GFS
AU  - Perret,N
AU  - Katsoulidis,AP
AU  - Chadwick,FM
AU  - Davies,RP
AU  - Haynes,A
AU  - Brammer,L
AU  - Weller,AS
AU  - Xiao,J
AU  - Rosseinsky,MJ
DO  - 10.1039/c5sc03494a
EP  - 2050
PY  - 2016///
SN  - 2041-6539
SP  - 2037
TI  - Encapsulation of an organometallic cationic catalyst by direct exchange into an anionic MOF
T2  - Chemical Science
UR  - http://dx.doi.org/10.1039/c5sc03494a
UR  - http://hdl.handle.net/10044/1/32630
VL  - 7
ER  -
Download