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A joint mechanism for singlet oxygen generation by diketone-anchored MIL-101: Exciton-mediated energy transfer and photosensitization
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2021-09-11 , DOI: 10.1016/j.apcata.2021.118360
Wentao Zhang 1 , Kunrui Wei 1 , Wenguang Huang 1 , Jianghua Yang 1 , Yonghai Gan 1 , Shujuan Zhang 1
Affiliation  

Post-synthetic modification with β-diketone has been proven as an effective strategy to improve the visible light response activities of metal-organic frameworks (MOFs). Nevertheless, the effects of the anchored-diketones on the excitonic behaviors and photocatalytic mechanisms of MOFs are still unclear. Herein, two MOFs (MIL-101 with CrIII and MIL-101 with AlIII) were employed as prototypical materials to further understand this post-synthetic modification strategy. Diketone anchoring could enhance the photocatalytic generation of singlet oxygen (1O2) by the two MOFs in a joint mechanism: exciton-mediated energy transfer and photosensitization. Diketone anchoring induced triplet exciton was found playing an important role in the photocatalytic generation of 1O2. The photosensitization of the anchored-diketone also played a key role in the photocatalytic generation of 1O2. The results here provide a useful guidance for the development of MOFs-based photocatalysts and are helpful to realize the regulation of excitonic behaviors and photocatalytic mechanisms of MOFs.



中文翻译:

二酮锚定的 MIL-101 产生单线态氧的联合机制:激子介导的能量转移和光敏化

β-二酮的合成后修饰已被证明是提高金属有机骨架(MOFs)可见光响应活性的有效策略。然而,锚定二酮对MOFs激子行为和光催化机制的影响仍不清楚。在此,两种 MOF(带有 Cr III 的MIL-101 和带有 Al III 的MIL-101 )被用作原型材料,以进一步了解这种合成后的改性策略。二酮锚定可以增强单线态氧(1 O 2) 由两个 MOF 联合机制:激子介导的能量转移和光敏化。发现二酮锚定诱导的三重态激子在光催化生成1 O 2 中起重要作用。锚定二酮的光敏化也在光催化生成1 O 2 中发挥了关键作用。该研究结果为MOFs基光催化剂的开发提供了有益的指导,有助于实现MOFs激子行为和光催化机制的调控。

更新日期:2021-09-24
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