Heteroleptic copper(I) photosensitizers of dibenzo[b,j]-1,10-phenanthroline derivatives driven hydrogen generation from water reduction
Heteroleptic copper(I) photosensitizers of dibenzo[b,j]-1,10-phenanthroline derivatives driven hydrogen generation from water reduction
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二苯并[b,j]-1,10-菲咯啉衍生物的杂配铜(I)光敏剂驱动水还原产氢
DOI：
10.1016/j.dyepig.2016.07.040
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发表时间：
2016-11
影响因子：
4.5
通讯作者：
Qing-An Wu
中科院分区：
文献类型：
--
作者：
Shu-Ping Luo;Nan-Yu Chen;Yuan-Yuan Sun;Liang-Min Xia;Zhi-Cai Wu;Henrik Junge;Matthias Beller;Qing-An Wu
合成了一系列二苯并[B，j]-1，10-菲咯啉氮配体，并原位合成了它们的铜配合物。并将其作为光敏剂应用于光催化Cu-Fe水还原体系中。在所测试的光敏剂中，以噻吨膦为P配体，5，8-二苯基-6，7-二氢二苯并[B，j] [1，10]菲咯啉为N配体的光敏剂是最有效的光敏剂。铜的最高转化数可达441，体系稳定性可达15 h。光物理和电子化学性质表明，铜配合物的激发时间较长是其光敏活性较高的原因。通过理论计算证明了配体间的电荷转移是主要的能量转移方式。值得注意的是，首次可以检测到并解释为什么菲咯啉的6，7位上的C-C单键可以显著提高光转换效率。这是由于较低的N配体的HOMO和较宽的能隙的贡献。
A series of dibenzo[b,j]-1,10-phenanthroline derivatives as N ligands was synthesized and their heteroleptic copper complexes obtained in-situ. These were applied as photosensitizer in photocatalyticCu-Fe water reduction system. Thixantphos as P ligand and 5,8-diphenyl-6,7-dihydrodibenzo[b,j] [1,10]phenanthroline as N ligands constitutes the most efficient photosensitizer among the tested photosensitizer. The highest turnover number of copper was up to 441 and the system achieved a stability of 15 h. Photophysical and electronic chemical character showed that the longer exited time of Cu complex is the reason for the higher photosensitive activity. By theoretical calculation it could be proven that ligand-to-ligand charge transfer is the main energy transition method. Noteworthy, for the first time it could be detected and explained why a C-C single bond at 6,7 positions of phenanthroline could significantly increase the light conversion efficiency. This is a result of the lower N ligand contribution in HOMO and the wider energy gap.
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