期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 56, 期 2, 页码 510-514出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201608553
关键词
artificial photosynthesis; carbon nitrides; EPR spectroscopy; hydrogen evolution; stable radical
资金
- Deutsche Forschungsgemeinschaft [LO1801/1-1]
- ERC Starting Grant [639233]
- Max Planck Society
- cluster of excellence Nanosystems Initiative Munich (NIM)
- Center for Nanoscience (CeNS)
- Christian Doppler Research Association (Austrian Federal Ministry of Science, Research and Economy, National Foundation for Research, Technology and Development)
- OMV Group
While natural photosynthesis serves as the model system for efficient charge separation and decoupling of redox reactions, bio-inspired artificial systems typically lack applicability owing to synthetic challenges and structural complexity. We present herein a simple and inexpensive system that, under solar irradiation, forms highly reductive radicals in the presence of an electron donor, with lifetimes exceeding the diurnal cycle. This radical species is formed within a cyanamide- functionalized polymeric network of heptazine units and can give off its trapped electrons in the dark to yield H-2, triggered by a co-catalyst, thus enabling the temporal decoupling of the light and dark reactions of photocatalytic hydrogen production through the radical's longevity. The system introduced here thus demonstrates a new approach for storing sunlight as long-lived radicals, and provides the structural basis for designing photocatalysts with long-lived photo-induced states.
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