Structure-Activated Copper Photosensitisers for Photocatalytic Water Reduction

被引:43
作者
Chen, Nan-Yu [1 ]
Xia, Liang-Min [1 ]
Lennox, Alastair J. J. [2 ]
Sun, Yuan-Yuan [1 ]
Chen, Hao [1 ]
Jin, Hai-Ming [1 ]
Junge, Henrik [2 ]
Wu, Qin-An [1 ]
Jia, Jian-Hong [1 ]
Beller, Matthias [2 ]
Luo, Shu-Ping [1 ]
机构
[1] Zhejiang Univ Technol, State Key Lab Breeding Base Green Chem Synth Tech, Chaowang Rd 18, Hangzhou 310014, Zhejiang, Peoples R China
[2] Univ Rostock eV, Leibniz Inst Katalyse, Albert Einstein Str 29a, D-18059 Rostock, Germany
关键词
copper; hydrogen; N ligands; photosensitisers; reduction; water chemistry; METAL-FREE SYSTEM; MG CHLOROPHYLL-A; HYDROGEN-PRODUCTION; COMPLEXES; EFFICIENT; LIGAND; SUBSTITUENT; DESIGN; DERIVATIVES; AMINATIONS;
D O I
10.1002/chem.201602598
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A series of phenanthroline-based ligands have been synthesised and their influence as bidentate nitrogen ligands in heteroleptic [Cu(P<^>P)(N<^>N)](+) photosensitisers in light-driven water reduction has been studied. In this noble-metal-free Cu-Fe-based photocatalytic water reduction system, the structural effects of the nitrogen ligands have been explored, including the steric and electronic effects of substituents at the 2,9- and 4,7-positions of phenanthroline. Ligands were prepared that led to increased hydrogen generation, with turnover numbers (TONCu) of up to 1388 being observed. All the new complexes were electrochemically and photophysically characterised. We demonstrate for the first time that the presence of fluorine in nitrogen ligands increases the efficacy of copper complexes in photocatalytic hydrogen production.
引用
收藏
页码:3631 / 3636
页数:6
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