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

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

10 Scopus citations

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.

Original languageEnglish (US)
Pages (from-to)10842-10846
Number of pages5
JournalDalton Transactions
Volume47
Issue number32
DOIs
StatePublished - 2018

Funding

This work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract DE-AC02-06CH11357 (Argonne National Laboratory). Use of the Advanced Photon Source is supported by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences, under Contract DE-AC02-06CH11357. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. DFT calculations were performed using the computational resources at the Argonne National Laboratory (ANL), Center for Nanoscale Materials (CNM) and resources provided by the Laboratory Computing Resource Center (LCRC) at ANL. H. K. acknowledges Dr Emily Carino for the use of the Raman microscope.

ASJC Scopus subject areas

  • Inorganic Chemistry

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