A Joint Mechanism for Singlet Oxygen Generation by Diketone-Anchored MIL-101: Exciton-mediated Energy Transfer and Photosensitization

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Abstract

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.

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Key words

Acetylacetone,Charge transfer,Exciton,Oxygen vacancy,Singlet oxygen

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Pretraining has recently greatly promoted the development of natural language processing (NLP)
We show that M6 outperforms the baselines in multimodal downstream tasks, and the large M6 with 10 parameters can reach a better performance
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The model is scaled to large model with 10 billion parameters with sophisticated deployment, and the 10 -parameter M6-large is the largest pretrained model in Chinese
Experimental results show that our proposed M6 outperforms the baseline in a number of downstream tasks concerning both single modality and multiple modalities We will continue the pretraining of extremely large models by increasing data to explore the limit of its performance

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