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Superoxide generated by blue light photocatalysis of g-C3N4/TiO2 for selective conversion of amines
Environmental Research ( IF 7.7 ) Pub Date : 2021-02-06 , DOI: 10.1016/j.envres.2021.110851
Xia Li , Shaoshuai Lyu , Xianjun Lang

Reactive oxygen species (ROS) are remarkably reactive chemical oxygen-containing molecules that not only occupy critical positions in cell signaling and homeostasis for regulating aerobic living organism's growth and development but also broadly participate in the environmental management as extraordinary oxidizing agents. Inspired by the behaviors of ROS, we designed an artful visible light photocatalytic system for the selective conversion of amines due to the activation of oxygen (O2) to superoxide (O2radical dot) over g-C3N4/TiO2. Here, blue light was manipulated as a light source to circumvent the initiation of the strong nonselective hydroxyl radical (radical dotOH) that is often generated by valence band holes (hvb+) of TiO2. Aerial O2 was employed to achieve the long-lived, exclusive ROS, O2radical dot, while acetonitrile, an aprotic solvent, was utilized to prolong the lifetime of O2radical dot. Importantly, the g-C3N4/TiO2 possesses an exceptional capability for the generation of O2radical dot. Based on the synergistic effect of two ingredients of the g-C3N4/TiO2 photocatalyst, the highly selective conversion of amines was achieved with superior conversions in comparison with the pristine TiO2 and g-C3N4. Furthermore, a mechanism dominated by O2radical dot was proposed according to the kinetic studies, electron paramagnetic resonance (EPR), and ROS quenching experiments. This work highlights the importance of ROS in defining the desirable outcomes over semiconductor photocatalysts.



中文翻译:

gC 3 N 4 / TiO 2的蓝光催化产生的超氧化物用于胺的选择性转化

活性氧(ROS)是非常活泼的化学含氧分子,它们不仅在细胞信号传导和体内平衡中占据重要位置,以调节有氧生物的生长和发育,而且作为非常规氧化剂广泛参与环境管理。由活性氧的行为的启发,我们设计了用于胺的选择性转化一个巧妙的可见光的光催化系统由于氧气(O的活化2)超氧化物(O 2 激进点- )在GC 3 Ñ 4 /二氧化钛2。在这里,将蓝光作为光源来规避强烈的非选择性羟基自由基(激进点OH)通常是由TiO 2的价带孔(h vb +)产生的。天线ø 2被使用,以实现长寿命,排他性ROS,O- 2 - 而乙腈,质子惰性的溶剂,用于延长的O-寿命2 - 。重要的是,GC 3 Ñ 4 /二氧化钛2具有为的O-产生一个特殊的能力2 - 。基于两种成分的gC 3 N 4 / TiO 2的协同作用激进点激进点激进点作为光催化剂,与原始的TiO 2和gC 3 N 4相比,胺的高选择性转化率更高。此外,机构被O为主2 激进点-根据动力学研究提出,电子顺磁共振(EPR),和ROS淬火实验。这项工作凸显了ROS在定义优于半导体光催化剂的理想结果方面的重要性。

更新日期:2021-02-15
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