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首页> 外文期刊>RSC Advances >The dependence of oxygen sensitivity on the molecular structures of Ir(iii) complexes and their application for photostable and reversible luminescent oxygen sensing
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The dependence of oxygen sensitivity on the molecular structures of Ir(iii) complexes and their application for photostable and reversible luminescent oxygen sensing

机译：氧敏感度对IR（III）复合物分子结构及其对光稳定和可逆发光氧气感应的依赖性的依赖性及其应用

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Three Ir( III ) complexes IrC1 , IrC2 , and IrC3 substituted with 4-(diphenylamino)phenyl (TPA), 4-(9 H -carbazol-9-yl)phenyl (Cz1), and 9-phenyl-9 H -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 I _(0) / I _(100) of 168.6 and K ~(app) _(SV) 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 σ _(IrC1) / σ _(Ir(ppy) _(3) ) , 1.24 ± 0.06 for σ _(IrC2) / σ _(Ir(ppy) _(3) ) , and 1.54 ± 0.08 for σ _(IrC3) / σ _(Ir(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 ( R ~(2) = 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.
机译：三烯（III）复合物IRC1，IRC2和IRC3被4-（二苯基氨基）苯基（TPA），4-（9h-Carbazol-9-基）苯基（CZ1）和9-苯基-9H-Carbazol取代制备-3-Y1（CZ2）部分并完全表征为磷光发射器。与IR（PPY）相比（PPY）_（3），TPA，CZ1和CZ2部分的引入强烈改善了IRC1-IRC3的氧敏感性。具有168.6和K〜（APP）_（SV）的I _（0）/ I _（100）的短衰减IRC1，THF中的氧气〜（α1）的_（SV）呈现最高的氧气灵敏度。 TPA和CZ部分引起了IR（III）复合物的显着碰撞半径变化，Σ_（IRC1）/Σ_（IR（PPY）_（3）），1.24±0.06，σ_（IRC2）/ Σ_（IR（ppy）_（3）），σ_（IRC3）/Σ_（IR（PPY）_（3）））和1.54±0.08。为了证明氧敏感性对氧敏感探针（OSPS）的分子结构的依赖性，首次施加旋转群（DSP）的临床化以确认IR（III）复合物的碰撞半径变化。在TPA，CZ1和CZ2部分上发现了显着的DSP，分别为0.23210（11.61％），0.08862（4.43％）和0.13201（6.60％）的旋转群体（旋转群体的百分比）。在TPA和CZ部分上的碰撞半径变化和旋转群之间的强烈线性相关性（R〜（2）= 0.997）是显而易见的。 DSP可用于描述氧敏感性对OSP的分子结构的依赖性。为了实现实时氧气感测，研究了固定在乙基纤维素（EC）中的IRC1-IRC3和IR（PPY）_（3）的光稳定性，氧气感测性能和操作稳定性。 IRC1 -EC薄膜在60分钟的照射和优异的连续氧监测操作稳定性后表现出优异的光稳定性，而连续氧监测没有衰减在4000秒内的原始发射强度。本研究定量并分析了氧敏感性对IR（III）复合物的分子结构的依赖性首次，并说明了实现高效传感器的可行方法，用于实时监测氧气。

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