کد مقاله کد نشریه سال انتشار مقاله انگلیسی نسخه تمام متن
1276170 1497489 2014 11 صفحه PDF دانلود رایگان
عنوان انگلیسی مقاله ISI
Iron–iron hydrogenase active subunit covalently linking to organic chromophore for light-driven hydrogen evolution
موضوعات مرتبط
مهندسی و علوم پایه شیمی الکتروشیمی
پیش نمایش صفحه اول مقاله
Iron–iron hydrogenase active subunit covalently linking to organic chromophore for light-driven hydrogen evolution
چکیده انگلیسی


• We constructed a photocatalytic [FeFe]-H2ase mimic with organic photosensitizer.
• Light-driven ET was revealed by steady-state spectroscopy and electrochemistry.
• The reduced [FeIFe0] species was further confirmed by laser flash photolysis.
• The photocatalyst catalyzed the H2 production with a remarkable TON of 24.2.

The first photocatalytic [FeFe]-hydrogenase ([FeFe]-H2ase) mimic 3 with noble-metal-free benzothiazole as donating photosensitizer had been successfully constructed via an easily accessible approach, and fully characterized by various spectroscopic and X-ray crystallographic techniques. Steady-state spectroscopy and electrochemistry revealed the evidences indicating that the photo-induced electron transfer occurred in 3. The reduced [FeIFe0] species was further confirmed by laser flash photolysis and considered to be responsible for the light-driven H2 evolution. As a result, the photocatalytic system consisting of the photocatalyst 3 and the sacrificial electron donor in the presence of proton source indeed produced H2 with a turnover number (TON) of 24.2 under light irradiation. The TON indicated a remarkably photocatalytic efficiency for an [FeFe]-H2ase mimic assembled by the covalent combination of a photosensitizer to the catalytic center. The results demonstrated the tremendous potential of present synthetic strategy for the construction of compact, inexpensive, easily accessible [FeFe]-H2ase model complexes as photocatalysts.

ناشر
Database: Elsevier - ScienceDirect (ساینس دایرکت)
Journal: International Journal of Hydrogen Energy - Volume 39, Issue 20, 3 July 2014, Pages 10434–10444
نویسندگان
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