Shellaiah Muthaiah, Thirumalaivasan Natesan, Aazaad Basheer, Awasthi Kamlesh, Sun Kien Wen, Wu Shu-Pao, Lin Ming-Chang, Ohta Nobuhiro
Department of Applied Chemistry, National Chiao Tung University, Hsinchu 300, Taiwan.
Center for Interdisciplinary Molecular Science, Department of Applied Chemistry, National Chiao Tung University, Hsinchu 300, Taiwan; Center for Emergent Functional Matter Science, National Chiao Tung University, Hsinchu 300, Taiwan.
Spectrochim Acta A Mol Biomol Spectrosc. 2020 Dec 5;242:118757. doi: 10.1016/j.saa.2020.118757. Epub 2020 Aug 1.
A novel rhodamine-pyridine conjugated spectroscopic probe RhP was synthesized and its X-ray single crystalline properties were revealed with tabulation. The RhP displayed a distinct pale-pink colorimetric and "turn-on" fluorescent response to Fe in aqueous media [HO:DMSO (95:5, v/v)] than that of other interfering ions. During the Fe recognition, the absorption (UV-Vis) and photoluminescence (PL) spectral studies revealed new peaks at 561 and 592 nm, respectively. The 1:1 stoichiometry and binding sites were verified by Job's plot, ESI-mass, and H NMR titrations. Subsequently, LOD and binding constant for RhP + Fe complex were estimated as 102.3 nM and 6.265 × 10 M from linear fitting and Benesi-Hildebrand plots, correspondingly. Sensor reversibility of RhP + Fe by EDTA was demonstrated by UV/PL and TRPL investigations. Moreover, the photoinduced energy transfer mechanism and band gap changes were established from the DFT interrogations. Lastly, cellular imaging studies were carried out to authenticate the real applicability of RhP in Fe detection.
合成了一种新型罗丹明-吡啶共轭光谱探针RhP,并通过列表揭示了其X射线单晶性质。与其他干扰离子相比,RhP在水介质[HO:DMSO(95:5,v/v)]中对Fe表现出明显的淡粉色比色和“开启”荧光响应。在Fe识别过程中,吸收(紫外-可见)光谱和光致发光(PL)光谱研究分别在561和592nm处发现了新峰。通过Job曲线、电喷雾电离质谱和核磁共振氢谱滴定验证了1:1的化学计量比和结合位点。随后,通过线性拟合和Benesi-Hildebrand曲线分别估计RhP+Fe配合物的检测限和结合常数为102.3 nM和6.265×10 M。通过紫外/PL和时间分辨光致发光研究证明了RhP+Fe被乙二胺四乙酸的传感器可逆性。此外,通过密度泛函理论研究确定了光诱导能量转移机制和带隙变化。最后,进行了细胞成像研究,以验证RhP在Fe检测中的实际适用性。