University of Sussex
Browse
__smbhome.uscs.susx.ac.uk_tjk30_Documents_Accepted Manuscript.pdf (674.27 kB)

Ethene activation and catalytic hydrogenation by a low-valent uranium pentalene complex

Download (674.27 kB)
journal contribution
posted on 2023-06-09, 20:02 authored by Nikolaos Tsoureas, Laurent Maron, Alexander F R Kilpatrick, Richard LayfieldRichard Layfield, Geoff Cloke
The reaction of the uranium(III) complex [U(?8-Pn††)(?5-Cp*)] (1) (Pn†† = C8H4(1,4-SiiPr3)2, Cp* = C5Me5) with ethene at atmospheric pressure produces the ethene-bridged diuranium complex [{(?8-Pn††)(?5-Cp*)U}2(µ-?2:?2-C2H4)] (2). A computational analysis of 2 revealed that coordination of ethene to uranium reduces the carbon–carbon bond order from 2 to a value consistent with a single bond, with a concomitant change in the formal uranium oxidation state from +3 in 1 to +4 in 2. Furthermore, the uranium–ethene bonding in 2 is of the d type, with the dominant uranium contribution being from f–d hybrid orbitals. Complex 2 reacts with hydrogen to produce ethane and reform 1, leading to the discovery that complex 1 also catalyzes the hydrogenation of ethene under ambient conditions.

Funding

EPSRC; EP/M023885/1

RadMag; ERC; 646740

History

Publication status

  • Published

File Version

  • Accepted version

Journal

Journal of the American Chemical Society

ISSN

0002-7863

Publisher

American Chemical Society

Issue

1

Volume

142

Page range

89-92

Department affiliated with

  • Chemistry Publications

Full text available

  • Yes

Peer reviewed?

  • Yes

Legacy Posted Date

2020-01-02

First Open Access (FOA) Date

2020-12-20

First Compliant Deposit (FCD) Date

2019-12-23

Usage metrics

    University of Sussex (Publications)

    Categories

    No categories selected

    Exports

    RefWorks
    BibTeX
    Ref. manager
    Endnote
    DataCite
    NLM
    DC