期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 12, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202215540
关键词
Cocrystal; Oxidation of Hydrocarbons; Photocatalysis; Polyoxotitanium Clusters; TiO2
资金
- NSFC
- Anhui Provincial Natural Science Foundation
- Key Project of Youth Elite Support Plan in Universities of Anhui Province
- Shaanxi Provincial Natural Science Foundation
- [91961106]
- [51902253]
- [21725102]
- [2108085MB46]
- [gxyqZD2021121]
- [2020JQ-778]
This study presents an atomically precise material model for photocatalysis, which incorporates Fe species into polyoxotitanium cluster to form a heterometallic Ti4Fe1 cocrystal. This cocrystal cluster effectively controls the energy and charge transfer, allowing the synergistic process of C(sp(3))-H bond activation by photogenerated holes and reactions by singlet oxygen. The Ti4Fe1 cluster achieves efficient and selective oxidation of hydrocarbons, outperforming Fe-doped Ti3Fe1 cluster in terms of conversion rate.
Photocatalysis is a promising yet challenging approach for the selective oxidation of hydrocarbons to valuable oxygenated chemicals with O-2 under mild conditions. In this work, we report an atomically precise material model to address this challenge. The key to our solution is the rational incorporation of Fe species into polyoxotitanium cluster to form a heterometallic Ti4Fe1 cocrystal. This newly designed cocrystal cluster, which well governs the energy and charge transfer as evidenced by spectroscopic characterizations and theoretical calculations, enables the synergistic process involving C(sp(3))-H bond activation by photogenerated holes and further reactions by singlet oxygen (O-1(2)). Remarkably, the cocrystal Ti4Fe1 cluster achieves efficient and selective oxidation of hydrocarbons (C-5 to C-16) into aldehydes and ketones with a conversion rate up to 12 860 mu mol g(-1) h(-1), 5 times higher than that of Fe-doped Ti3Fe1 cluster. This work provides insights into photocatalyst design at atomic level enabling synergistic catalysis.
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