期刊
DALTON TRANSACTIONS
卷 42, 期 41, 页码 14883-14891出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c3dt51849c
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资金
- North Carolina State University
- North Carolina Biotechnology Center
- NCSU Department of Chemistry
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001011]
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.
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