Nuclearity effects in supported, single-site Fe(II) hydrogenation pre-catalysts

Ryan R. Langeslay; Hyuntae Sohn; Bo Hu; Jacob S. Mohar; Magali Ferrandon; Cong Liu; Hacksung Kim; A. Jeremy Kropf; Ce Yang; Jens Niklas; Oleg G. Poluektov; E. Ercan Alp; Patricia Ignacio-de Leon; Alfred P. Sattelberger; Adam S. Hock; Massimiliano Delferro

doi:10.1039/C8DT02720J

Nuclearity effects in supported, single-site Fe(ii) hydrogenation pre-catalysts†‡

Ryan R. Langeslay,

*^a Hyuntae Sohn,^a Bo Hu,^ab Jacob S. Mohar,^a Magali Ferrandon,^a Cong Liu,^a Hacksung Kim,^ac A. Jeremy Kropf,^a Ce Yang,

^a Jens Niklas,

^a Oleg G. Poluektov,

^a E. Ercan Alp,^d Patricia Ignacio-de Leon,^e Alfred P. Sattelberger,*^a Adam S. Hock*^ab and Massimiliano Delferro

*^a

Author affiliations

* Corresponding authors

^a Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL 60439, USA
E-mail: langesrr@anl.gov, asattelberger@anl.gov, delferro@anl.gov

^b Department of Chemistry, Illinois Institute of Technology, Chicago, IL 60616, USA
E-mail: ahock@iit.edu

^c Catalysis Center, Northwestern University, Evanston, IL 60208, USA

^d X-ray Science Division, Argonne National Laboratory, Lemont, IL 60439, USA

^e Energy Sciences Division, Argonne National Laboratory, Lemont, IL 60439, USA

Abstract

Dimeric and monomeric supported single-site Fe(II) pre-catalysts on SiO₂ have been prepared via organometallic grafting and characterized with advanced spectroscopic techniques. Manipulation of the surface hydroxyl concentration on the support influences monomer/dimer formation. While both pre-catalysts are highly active in liquid-phase hydrogenation, the dimeric pre-catalyst is ∼3× faster than the monomer. Preliminary XAS experiments on the H₂-activated samples suggest the active species are isolated Fe(II) sites.

This article is part of the themed collection: In celebration of Richard Andersen’s 75th birthday

Dalton Transactions

Nuclearity effects in supported, single-site Fe(ii) hydrogenation pre-catalysts†‡

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Nuclearity effects in supported, single-site Fe(II) hydrogenation pre-catalysts

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