Lin Tzu-Pin, Chen Chan-Yu, Wen Yuh-Sheng, Sun Shih-Sheng
Institute of Chemistry, Academia Sinica, Nankang, Taipei 115, Taiwan, Republic of China.
Inorg Chem. 2007 Oct 29;46(22):9201-12. doi: 10.1021/ic701300a. Epub 2007 Sep 15.
We report the synthesis, characterization, and photophysical properties of a series of organic receptors and their corresponding ReI and RuII metal complexes as anion probes featuring bis(sulfonamide) interacting sites incorporating highly chromophoric pi-conjugated quinoxaline moieties. The interactions with various anions were extensively investigated. These probe molecules are capable of recognizing F-, OAc-, CN-, and H2PO4- with different sensitivities. The probe-anion interactions can be easily visualized via naked-eye colorimetric or luminescent responses. Probe 1 has the weakest acidic sulfonamide N-H protons and therefore simply forms hydrogen-bonding complexes with F-, OAc-, CN-, and H2PO4-. Probe 2 undergoes a stepwise process with the addition of F- and OAc-: formation of a hydrogen-bound complex followed by sulfonamide N-H deprotonation. Direct sulfonamide N-H deprotonation occurs upon the addition of CN-, while only a hydrogen-bound complex forms with the H2PO4- ion for probe 2 in a dimethyl sulfoxide (DMSO) solution. Similar probe-anion interactions occur in probe 3 with the addition of F-, CN-, or H2PO4-. However, only a genuine hydrogen-bound complex forms in the presence of the OAc- ion in a DMSO solution of probe 3 because of the subtle difference in the pKa values of sulfonamide N-H protons when probes 2 and 3 are compared. Coordination of probe 1 to a ReI center or probe 2 to a RuII center increases the intrinsic acidity of sulfonamide N-H protons and results in an enhanced sensitivity to anions.
我们报道了一系列有机受体及其相应的铼(I)和钌(II)金属配合物的合成、表征和光物理性质,这些化合物作为阴离子探针,具有双(磺酰胺)相互作用位点,并结合了发色性很强的π共轭喹喔啉部分。对它们与各种阴离子的相互作用进行了广泛研究。这些探针分子能够以不同的灵敏度识别氟离子(F-)、醋酸根离子(OAc-)、氰根离子(CN-)和磷酸二氢根离子(H2PO4-)。探针与阴离子的相互作用可以通过肉眼比色或发光响应轻松观察到。探针1的磺酰胺N-H质子酸性最弱,因此仅与F-、OAc-、CN-和H2PO4-形成氢键复合物。探针2在加入F-和OAc-时经历一个逐步过程:先形成氢键复合物,随后磺酰胺N-H去质子化。加入CN-时直接发生磺酰胺N-H去质子化,而在二甲基亚砜(DMSO)溶液中,对于探针2,H2PO4-离子仅形成氢键复合物。在探针3中加入F-、CN-或H2PO4-时也会发生类似的探针-阴离子相互作用。然而,由于比较探针2和3时磺酰胺N-H质子的pKa值存在细微差异,在探针3的DMSO溶液中,仅在醋酸根离子存在时形成真正的氢键复合物。探针1与铼(I)中心配位或探针2与钌(II)中心配位会增加磺酰胺N-H质子的固有酸度,并导致对阴离子的灵敏度增强。