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Supported CuII Single-Ion Catalyst for Total Carbon Utilization of C2 and C3 Biomass-Based Platform Molecules in the N-Formylation of Amines
Authors
Angelika Brückner
Xingchao Dai
+4 more
Carsten Kreyenschulte
Jabor Rabeah
Feng Shi
Xinzhi Wang
Publication date
1 January 2021
Publisher
Weinheim : Wiley-VCH
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PubMed
Abstract
The shift from fossil carbon sources to renewable ones is vital for developing sustainable chemical processes to produce valuable chemicals. In this work, value-added formamides were synthesized in good yields by the reaction of amines with C2 and C3 biomass-based platform molecules such as glycolic acid, 1,3-dihydroxyacetone and glyceraldehyde. These feedstocks were selectively converted by catalysts based on Cu-containing zeolite 5A through the in situ formation of carbonyl-containing intermediates. To the best of our knowledge, this is the first example in which all the carbon atoms in biomass-based feedstocks could be amidated to produce formamide. Combined catalyst characterization results revealed preferably single CuII sites on the surface of Cu/5A, some of which form small clusters, but without direct linking via oxygen bridges. By combining the results of electron paramagnetic resonance (EPR) spin-trapping, operando attenuated total reflection (ATR) IR spectroscopy and control experiments, it was found that the formation of formamides might involve a HCOOH-like intermediate and .NHPh radicals, in which the selective formation of .OOH radicals might play a key role. © 2021 The Authors. Chemistry - A European Journal published by Wiley-VCH Gmb
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Repositorium für Naturwissenschaften und Technik
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oai:oa.tib.eu:123456789/8863
Last time updated on 23/07/2022
PubMed Central
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oai:pubmedcentral.nih.gov:9292...
Last time updated on 02/09/2022