Synthesis, characterization and structural investigation of novel meso-pyridyl BODIPY-cobaloxime complexes

被引:27
作者
Bartelmess, Juergen [1 ]
Weare, Walter W. [1 ]
Sommer, Roger D. [1 ]
机构
[1] N Carolina State Univ, Raleigh, NC 27695 USA
关键词
ARTIFICIAL PHOTOSYNTHESIS; HYDROGEN-PRODUCTION; ELECTRON-TRANSFER; CHARGE-TRANSFER; ENERGY-TRANSFER; WATER; MODELS; DYES; DISSOCIATION; PORPHYRIN;
D O I
10.1039/c3dt51849c
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
We report the synthesis of four boron-dipyrromethene (BODIPY) sensitized cobaloxime complexes as structural models of light-driven proton reduction catalysts. The BODIPY chromophore is covalently linked to the cobaloxime via a pyridine molecule in the meso-position of the BODIPY. Electron withdrawing or donating substituents on the pyridine (e.g. chloro-or methyl-groups) allow a comparison of the influence of these substituents on cobaloxime-BODIPY interactions. This includes altering the overall stability of the complexes and tuning the catalytically relevant CoII/III redox couple over a range of 220 mV, which will assist in the design of future cobaloxime-chromophore complexes. All complexes were characterized using electrochemistry, electronic absorption and fluorescence spectroscopy. Additionally, we present crystal structures of the four new BODIPY-cobaloxime complexes and elucidate the influence of the structural modifications. We found that these compounds produce sub-stoichiometric quantities of hydrogen under standard photon-driven hydrogen evolving conditions.
引用
收藏
页码:14883 / 14891
页数:9
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