Dark Photocatalysis: Storage of Solar Energy in Carbon Nitride for Time-Delayed Hydrogen Generation
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- 作者：Dr. Vincent Wing-hei Lau ; Dr. Daniel Klose ; Hatice Kasap ; Filip Podjaski ; Marie-Claire Pignié ; Dr. Erwin Reisner ; Prof. Gunnar Jeschke and Prof. Bettina V. Lotsch
- 刊名：Angewandte Chemie
- 出版年：2017
- 出版时间：January 9, 2017
- 年：2017
- 卷：129
- 期：2
- 页码：525-529
- 全文大小：2246K
- ISSN：1521-3757
文摘
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 H2, 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.