Abstract
1,4,7-Triazacyclononane (L) and its methylated analog (L‘) form complexes with zeolite-exchanged Mn2+, Co2+, or Cu2+. Through comparison with diluted solutions of the complexes, the effect of the zeolite environment on the complex formation was evaluated. In the case of Mn2+, the complexation was monitored by observing the zero-field splitting in the X- and Q-band ESR spectra of the Mn2+ ion. Adsorption of L into metal Y zeolites yields bis L complexes; the L‘ mono complexes are formed. The latter complexes are not coordinated by the zeolite surface, as deduced from the spectral parameters of the [Mn(L‘)]2+ and [Cu(L‘)]2+ complexes. Mono [Co(L‘)]2+ in the zeolite is a reversible dioxygen binder, a property not previously documented for these complexes in solution. Exposure of [Mn(L)2]2+ or [Mn(L‘)]2+ containing Y zeolites to H2O2 results in intraporous formation of oxidized Mn dimers. The constrained zeolite environment seems to stabilize the oxidized dimers of Mn and L by preventing further cluster expansion.
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