Photocatalytic Water Oxidation: Tuning Light-Induced Electron Transfer by Molecular Co4O4 Cores

被引:193
作者
Berardi, Serena [1 ,2 ]
La Ganga, Giuseppina [3 ,4 ]
Natali, Mirco [5 ,6 ]
Bazzan, Irene [1 ,2 ]
Puntoriero, Fausto [3 ,4 ]
Sartorel, Andrea [1 ,2 ]
Scandola, Franco [5 ,6 ]
Campagna, Sebastiano [3 ,4 ]
Bonchio, Marcella [1 ,2 ]
机构
[1] Univ Padua, ITM CNR, I-35131 Padua, Italy
[2] Univ Padua, Dept Chem Sci, I-35131 Padua, Italy
[3] Univ Messina, Dipartimento Chim Inorgan Chim Analit & Chim Fis, I-98166 Messina, Italy
[4] Ctr Interuniv Convers Chim Energia Solare, Sez Messina, I-98166 Messina, Italy
[5] Univ Ferrara, Dept Chem, I-44121 Ferrara, Italy
[6] Ctr Interuniv Convers Chim Energia Solare, Sez Ferrara, I-44121 Ferrara, Italy
关键词
OXYGEN-EVOLVING CATALYST; COBALT; PHOTOSYNTHESIS; MANGANESE; CLUSTERS; PLANET;
D O I
10.1021/ja303951z
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Isostructural cubane-shaped catalysts [Co-4(III)(mu-O)(4)(mu-CH3COO)(4)(p-NC5H4X)(4)], 1-X (X = H, Me, t-Bu, OMe, Br, COOMe, CN), enable water oxidation under dark and illuminated conditions, where the primary step of photoinduced electron transfer obeys to Hammett linear free energy relationship behavior. Ligand design and catalyst optimization are instrumental for sustained O-2 productivity with quantum efficiency up to 80% at lambda > 400 nm, thus opening a new perspective for in vitro molecular photosynthesis
引用
收藏
页码:11104 / 11107
页数:4
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