Reversible and cooperative photoactivation of single-atom Cu/TiO2 photocatalysts
Reversible and cooperative photoactivation of single-atom Cu/TiO2 photocatalysts
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DOI：
10.1038/s41563-019-0344-1
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发表时间：
2019-06-01
期刊：
影响因子：
41.2
通讯作者：
Hyeon, Taeghwan
中科院分区：
文献类型：
--
作者：
Lee, Byoung-Hoon;Park, Sunghak;Hyeon, Taeghwan
可逆协同活化过程是生物酶最重要的特征之一，它包括从周围氧化还原介质的电子转移、辅因子的可逆价态变化和宏观功能/结构变化，常用于均相催化剂的设计。然而，实际上没有关于具有这些酶样特征的工业上重要的多相催化剂的报道。在这里，我们报告的设计和合成的高活性二氧化钛光催化剂，将特定的单铜原子（Cu/二氧化钛），表现出可逆的和合作的光活化过程。我们的原子水平的设计和合成策略提供了一个平台，有利于价态控制的助催化剂铜原子，可逆调制的宏观光电性能的二氧化钛和光催化制氢活性的增强，扩展了传统的非均相催化剂的边界。
The reversible and cooperative activation process, which includes electron transfer from surrounding redox mediators, the reversible valence change of cofactors and macroscopic functional/structural change, is one of the most important characteristics of biological enzymes, and has frequently been used in the design of homogeneous catalysts. However, there are virtually no reports on industrially important heterogeneous catalysts with these enzyme-like characteristics. Here, we report on the design and synthesis of highly active TiO2 photocatalysts incorporating site-specific single copper atoms (Cu/TiO2) that exhibit a reversible and cooperative photoactivation process. Our atomic-level design and synthetic strategy provide a platform that facilitates valence control of co-catalyst copper atoms, reversible modulation of the macroscopic optoelectronic properties of TiO2 and enhancement of photocatalytic hydrogen generation activity, extending the boundaries of conventional heterogeneous catalysts.