Real-Time Visualization of Active Species in a Single-Site Metal–Organic Framework Photocatalyst
Real-Time Visualization of Active Species in a Single-Site Metal–Organic Framework Photocatalyst
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DOI：
10.1021/acsenergylett.8b00062
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发表时间：
2018-02
影响因子：
22
通讯作者：
Sizhuo Yang;B. Pattengale;Sungsik Lee;Jier Huang
中科院分区：
文献类型：
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作者：
Sizhuo Yang;B. Pattengale;Sungsik Lee;Jier Huang
在这项工作中，我们报道了一种新的单位点光催化剂（Co-Ru-UIO-67(bpy)），该催化剂基于金属-有机框架平台，结合了分子光敏剂和催化剂。我们发现，这种催化剂不仅在光驱动H2生产中表现出优异的活性，而且可以在不损失活性的情况下回收。利用光学瞬态吸收光谱和原位x射线吸收光谱相结合的方法，我们不仅捕获了加入的光敏剂在超快电荷转移后形成的关键CoI中间物质，而且确定了催化循环中的速率限制步骤，为深入了解这些单位点金属-有机框架光催化剂的催化机理提供了线索。
In this work, we report a new single-site photocatalyst (Co-Ru-UIO-67(bpy)) based on a metal–organic framework platform with incorporated molecular photosensitizer and catalyst. We show that this catalyst not only demonstrates exceptional activity for light-driven H2 production but also can be recycled without loss of activity. Using the combination of optical transient absorption spectroscopy and in situ X-ray absorption spectroscopy, we not only captured the key CoI intermediate species formed after ultrafast charge transfer from the incorporated photosensitizer but also identified the rate-limiting step in the catalytic cycle, providing insight into the catalysis mechanism of these single-site metal–organic framework photocatalysts.