RSC Advances p. 15370 - 15380 (2019)
Update date:2022-08-10
Topics:
Xing, Yang
Qiao, Chengfang
Li, Xinmin
Li, Chun
Wang, Honghao
Li, Fayun
Di, Ling
Yang, Zhanxu
Three Ir(iii) complexes IrC1, IrC2, and IrC3 substituted with 4-(diphenylamino)phenyl (TPA), 4-(9H-carbazol-9-yl)phenyl (Cz1), and 9-phenyl-9H-carbazol-3-yl (Cz2) moieties were prepared and fully characterized as phosphorescent emitters. In comparison with Ir(ppy)3, introduction of TPA, Cz1, and Cz2 moieties strongly improved the oxygen sensitivities of IrC1-IrC3. Short-decayed IrC1 with I0/I100 of 168.6 and KappSV of 202.2 bar-1 in THF exhibited the highest sensitivity for oxygen. TPA and Cz moieties caused remarkable collision radius variations of the Ir(iii) complexes with 2.13 ± 0.08 for σIrC1/σIr(ppy)3, 1.24 ± 0.06 for σIrC2σIr(ppy)3, and 1.54 ± 0.08 for σIrC3σIr(ppy)3. For demonstrating the dependence of oxygen sensitivity on the molecular structure of the oxygen-sensitive probes (OSPs), the delocalization of spin populations (DSPs) has been applied for the first time to confirm the collision radius variations of Ir(iii) complexes. Remarkable DSPs were found on the TPA, Cz1, and Cz2 moieties with the spin population (percentage of the spin population) of 0.23210 (11.61%), 0.08862 (4.43%), and 0.13201 (6.60%), respectively. And strong linear correlations (R2 = 0.997) between the collision radius variations and spin population on TPA and Cz moieties were apparent. The DSPs could be used to describe the dependence of oxygen sensitivity on the molecular structure of the OSPs. For achieving real-time oxygen sensing, the photostability, oxygen sensing performance, and operational stability of IrC1-IrC3 and Ir(ppy)3 immobilized in ethyl cellulose (EC) were investigated. The IrC1-EC film demonstrated outstanding photostability after 60 min of irradiation and excellent operational stability for continuous oxygen monitoring with no attenuation of the original emission intensity in 4000 s. This study quantified and analyzed the dependence of oxygen sensitivity on the molecular structure of Ir(iii) complexes for the first time and illustrated a feasible approach to achieve high-efficiency sensors for real-time monitoring of oxygen.
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