From haemoglobin to single-site hydrogenation catalyst
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Published version
Author(s)
Type
Journal Article
Abstract
Iron-based single-site catalysts hold immense potential for achieving highly selective chemical processes, with the added advantage of iron being an earth-abundant metal. They are widely explored in electrocatalysis for oxygen reduction and display promising catalytic activity for organic transformations. In particular, FeNx@C catalysts are active for the reduction of nitroarene into aromatic amines. Yet, they are difficult to mass-produce, and most preparation methods fail to avoid single site aggregation. Here we prepared FeNx@C catalysts from bio-derived compounds, xylose and haemoglobin, in a simple two-step process. Since haemoglobin naturally contains FeNx single-sites, we successfully repurposed them into hydrogenation catalytic centers and avoided their aggregation during the preparation of the material. Their single-site nature was demonstrated by aberration-corrected transmission electron microscopy and X-ray absorption techniques. They were shown to be active for transfer hydrogenation of nitroarenes into anilines, with excellent substrate selectivity and recyclability, as demonstrated by the preserved yield across seven catalytic cycles. We also showed that FeNx@C could be used to prepare 2-phenylbenzimidazole through a reduction/condensation tandem. Our work shows for the first time the viability of biomass precursors to prepare Fe single-site hydrogenation catalysts.
Date Issued
2022-10-07
Date Acceptance
2022-09-02
Citation
Green Chemistry, 2022, 24 (19), pp.7574-7583
ISSN
1463-9262
Publisher
Royal Society of Chemistry
Start Page
7574
End Page
7583
Journal / Book Title
Green Chemistry
Volume
24
Issue
19
Copyright Statement
This journal is © The Royal Society of Chemistry 2022. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.
License URL
Identifier
https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000851576200001&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=a2bf6146997ec60c407a63945d4e92bb
Subjects
CARBONIZED HEMOGLOBIN
CATHODE CATALYST
Chemistry
Chemistry, Multidisciplinary
EPR SPECTROSCOPY
Green & Sustainable Science & Technology
HYDROTHERMAL CARBONIZATION
IRON-OXIDE
NITROARENES
NITRO-COMPOUNDS
OXYGEN REDUCTION
Physical Sciences
PORE DEVELOPMENT
Science & Technology
Science & Technology - Other Topics
SELECTIVE HYDROGENATION
Publication Status
Published
Date Publish Online
2022-09-06