Photocatalytic water oxidation at soft interfaces

Photocatalytic water oxidation at soft interfaces
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DOI:
10.1039/c4sc01018c
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发表时间:
2014-01-01
期刊:
影响因子:
8.4
通讯作者:
Koenig, Burkhard
Koenig, Burkhard
中科院分区:
化学1区
文献类型:
--
作者:
Hansen, Malte;Li, Fei;Koenig, Burkhard

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分子水氧化催化剂首次与光敏剂共嵌入磷脂膜中。这些功能化的单层小囊泡在可见光照射下通过光催化产生分子氧。催化剂在脂水界面的二维组装模拟了生物中的光活性膜,并允许在500nm的极低催化剂浓度下光催化水氧化,这在均相系统中是无法达到的。在膜的主转变温度以下获得最高的吨,表明相分离,聚类和有限的动态增强了组装的光催化活性。膜共包埋的概念可应用于光敏剂和水氧化催化剂的各种组合、比例和浓度,为人工光合作用提供了新的途径。
Molecular water oxidation catalysts have been, for the first time, co-embedded with a photosensitizer into phospholipid membranes. The functionalized small unilamellar vesicles produce molecular oxygen by photocatalysis when irradiated with visible light in aqueous buffer. The two dimensional assembly of the catalysts at the lipid-water interface mimics photoactive membranes in biology and allows photocatalytic water oxidation at very low catalyst concentrations of 500 nM, which cannot be reached in homogeneous systems. Highest TONs are obtained below the membrane's main transition temperature indicating that phase separation, clustering and a limited dynamic enhance the photocatalytic activity of the assembly. The concept of membrane co- embedding can be applied to various combinations, ratios and concentrations of photosensitizers and water oxidizing catalysts, providing a new approach for artificial photosynthesis.