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Heteroleptic, polynuclear dysprosium($_{III}$)-carbamato complexes throughin situcarbon dioxide capture

Schlittenhardt, Sören; Moreno-Pineda, Eufemio; Ruben, Mario

Abstract:
Amine groups are among the most effective systems for carbon dioxide capture. Reminiscent of the activation of nature's most abundant enzyme RuBisCO, the treatment of amines with CO$_{2}$ in the presence of oxophilic metal ions, e.g. Mg$^{2+}$, results in the formation of carbamates. Here we report the synthesis, structure and magnetic properties of three new dysprosium-carbamato complexes. The reaction of gaseous CO$_{2}$ with N,N-diisopropylamine and DyCl$_{3}$(DME)$_{2}$ (DME = Dimethoxyethane) in toluene leads to the formation of the tetrametallic complex [Dy$_{4}$(O$_{2}$CNiPr$_{2}$)$_{10}$(O-C$_{2}$H$_{4}$–OMe)$_{2}$]. The addition of 2-hydroxy-3-methoxybenzaldehyde-N-methylimine yields the hexametallic compound [Dy$_{6}$(O$_{2}$CNiPr$_{2}$)$_{8}$(O-C$_{2}$H$_{4}$–OMe)$_{2}$(CO$_{3}$)$_{2}$(C$_{9}$O$_{2}$NH$_{10}$)$_{4}$] in which the metal sites form a chair-like configuration; The same hexanuclear motif is obtained using N,N-dibenzylamine. We show that by employing CO$_{2}$ as a feedstock, we are able to capture up to 2.5 molecules of CO$_{2}$ per Dy ion. Magnetic measurements show a decreasing χMT at low temperatures. Combining the experimental magnetic data with ab initio calculations reveils tilting of the easy axes and implies the presence of antiferromagnetic interactions between the Dy($_{III}$) metal ions.

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Verlagsausgabe §
DOI: 10.5445/IR/1000131391
Veröffentlicht am 16.04.2021
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Nanotechnologie (INT)
Institut für Quantenmaterialien und -technologien (IQMT)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2021
Sprache Englisch
Identifikator ISSN: 1477-9226, 0300-9246, 1470-479X, 1477-9234, 2050-5671
KITopen-ID: 1000131391
Erschienen in Dalton Transactions
Verlag Royal Society of Chemistry (RSC)
Band 50
Heft 13
Seiten 4735-4742
Nachgewiesen in Scopus
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