A new approach to the synthesis of heteronuclear propeller-like single molecule magnets

Pasquale Totaro; Kátia Cristina M. Westrup; Marie-Emmanuelle Boulon; Giovana G. Nunes; Davi F. Back; Andersson Barison; Samuele Ciattini; Matteo Mannini; Lorenzo Sorace; Jaísa F. Soares; Andrea Cornia; Roberta Sessoli

doi:10.1039/C2DT32618C

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Corresponding authors

Dipartimento di Chimica Ugo Schiff and INSTM RU, Università degli Studi di Firenze, Via della Lastruccia 3-13, 50019 Sesto Fiorentino-FI, Italy
E-mail: roberta.sessoli@unifi.it;
Fax: +0039 055 4573372 ;
Tel: +0039 055 4573268

Departamento de Química, Universidade Federal do Paraná, Centro Politécnico, Curitiba-PR, Brazil
E-mail: jaisa.soares@ufpr.br

Departamento de Química, Universidade Federal de Santa Maria, Camobi, Santa Maria-RS, Brazil

Dipartimento di Scienze Chimiche e Geologiche and INSTM RU, Università degli Studi di Modena e Reggio Emilia, Via G. Campi 183, 41100 Modena, Italy

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Propeller-like [Fe₄(L)₂(dk)₆] complexes, in which Hdk is a β-diketone and H₃L is a tripodal alcohol, R–C(CH₂OH)₃, exhibit tunable magnetic anisotropy barriers and retain their magnetic memory effect when chemically anchored on metal surfaces. Heteronuclear analogues of these M₄ complexes have been sought to afford a library of compounds with different total spin (S) values, but synthetic efforts described so far gave solid solutions containing M₄ in addition to the desired M₃M′ species. We now present a novel synthetic route to M₃M′ complexes featuring a central chromium(III) ion. The three-step preparation goes through coordination of Cr^III by two equivalents of tripodal alkoxide (R = Et and Ph), followed by reaction of this complex “core” with the peripheral +III metal ions. Products have been characterised by chemical analyses together with ¹H-NMR, FTIR, W-band EPR, DC/AC magnetic susceptibility measurements and single crystal X-ray diffractometry. Due to the chemical inertness of Cr^III, this route yields 100% pure Fe₃Cr complexes without metal scrambling; what is more, it is suitable for designing novel heteronuclear single molecule magnets (SMMs) with a variety of d- and f-metals and R groups.

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A new approach to the synthesis of heteronuclear propeller-like single molecule magnets

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