化学
荧光
离解(化学)
组氨酸
流离失所(心理学)
检出限
氨基酸
组合化学
纳米技术
化学传感器
工作(物理)
肽
生物物理学
生物传感器
光化学
能量学
选择性
作者
Zhizhong Zhao,Lijuan Liang,Xin Wang,Xi Zhang,Can Diao,Xiangyuan Yan,Pingru Su,Yu Tang
标识
DOI:10.1021/acs.inorgchem.6c02450
摘要
The rational control of ligand substitution in metal complexes remains underexplored for turn-on fluorescent probes. Here, varying the metal center (Co 2+, Ni 2+, or Cu 2+ ) in AIE-based complexes M(L) 2 (L = tetraphenylethylene-based β-diketone) enables precise tuning of metal–ligand bond dissociation, dictating competitive ligand exchange with histidine (His). Single-crystal X-ray diffraction confirmed the structures. All complexes are nonemissive in the aggregated state due to paramagnetic quenching. Upon His addition, only Ni(L) 2 undergoes rapid and complete ligand displacement, generating a strong fluorescence turn-on signal within 10 min at room temperature. Co(L) 2 reacts much more slowly (>560 min), while Cu(L) 2 shows no change. DFT calculations based on crystal structures quantify Gibbs free energy changes: spontaneous displacement in Ni(L) 2 correlates with favorable ligand dissociation energetics, whereas Cu(L) 2 is thermodynamically trapped. Exploiting this metal-dependent reactivity, Ni(L) 2 serves as a highly selective and rapid fluorescent probe for His, discriminating against 20 other amino acids with a detection limit of 4.66 nM. This work establishes a coordination chemistry strategy for designing small-molecule probes by modulating metal-dependent dissociation energetics in AIE complexes, moving beyond conventional PET mechanisms.
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