Bazzicalupi Carla, Bencini Andrea, Berni Emanuela, Bianchi Antonio, Borsari Lucia, Giorgi Claudia, Valtancoli Barbara, Lodeiro Carlos, Lima João Carlos, Parola A Jorge, Pina Fernando
Dipartimento di Chimica, Polo Scientifico, Università di Firenze, Via della Lastruccia 3, 50019 Sesto Fiorentino, Firenze, Italy.
Dalton Trans. 2004 Feb 21(4):591-7. doi: 10.1039/b315608g. Epub 2004 Jan 26.
Protonation and Zn(II), Cd(II) and Hg(II) coordination with the ligand 5-aminoethyl-2,5,8-triaza-[9]-10,23-phenanthrolinophane (L2), which contains an aminoethyl pendant attached to a phenanthroline-containing macrocycle, have been investigated by means of potentiometric, 1H NMR and spectrofluorimetric titrations in aqueous solutions. The coordination properties of L2 are compared with those of the ligand 2,5,8-triaza-[9]-10,23-phenanthrolinophane (L1). Ligand protonation occurs on the aliphatic amine groups and does not involve directly the heteroaromatic nitrogens. The fluorescence emission properties of L2 are controlled by the protonation state of the benzylic nitrogens: when not protonated, their lone pairs are available for an electron transfer process to the excited phenanthroline, quenching the emission. As a consequence, the ligand is emissive only in the highly charged [H3L2]3+ and [H4L2]4+ species, where the benzylic nitrogens are protonated. Considering metal complexation, both [ML1]2+ and [ML2]2+ complexes (M = Zn(II) and Cd(II)) are not emissive, since the benzylic nitrogens are weakly involved in metal coordination, and, once again, they are available for quenching the fluorescence emission. Protonation of the L2 complexes to give [MHL2]3+ species, instead, leads to a recovery of the fluorescence emission. Complex protonation, in fact, occurs on the ethylamino group and gives a marked change of the coordination sphere of the metals, with a stronger involvement in metal coordination of the benzylic nitrogens; consequently, their lone pairs are not available for the process of emission quenching.
通过电位滴定法、¹H NMR和荧光光谱滴定法,研究了配体5-氨基乙基-2,5,8-三氮杂-[9]-10,23-菲咯啉环烷(L2)的质子化以及锌(II)、镉(II)和汞(II)与该配体的配位情况,该配体含有连接在含菲咯啉大环上的氨基乙基亚甲基链。将L2的配位性质与配体2,5,8-三氮杂-[9]-10,23-菲咯啉环烷(L1)的配位性质进行了比较。配体质子化发生在脂肪胺基团上,并不直接涉及杂芳环氮原子。L2的荧光发射性质受苄基氮原子质子化状态的控制:当未质子化时,它们的孤对电子可用于向激发态菲咯啉进行电子转移过程,从而淬灭发射。因此,该配体仅在苄基氮原子质子化的高电荷[H₃L2]³⁺和[H₄L2]⁴⁺物种中发射荧光。考虑到金属络合,[ML1]²⁺和[ML2]²⁺络合物(M = 锌(II)和镉(II))均不发射荧光,因为苄基氮原子很少参与金属配位作用,并且它们再次可用于淬灭荧光发射。相反,将L2络合物质子化生成[MHL2]³⁺物种会导致荧光发射恢复。实际上,络合物质子化发生在乙氨基上,并使金属的配位球发生显著变化,苄基氮原子对金属配位的参与度更高;因此,它们的孤对电子不可用于发射淬灭过程。