Porphyrin-based Ti-MOFs conferred with single-atom Pt for enhanced photocatalytic hydrogen evolution and NO removal
Porphyrin-based Ti-MOFs conferred with single-atom Pt for enhanced photocatalytic hydrogen evolution and NO removal
复制标题
卟啉基 Ti-MOF 赋予单原子 Pt 以增强光催化析氢和 NO 去除
DOI：
10.1016/j.cej.2021.132045
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发表时间：
2021-09-02
影响因子：
15.1
通讯作者：
He, Youzhou
中科院分区：
文献类型：
--
作者：
Feng, Huan;Li, Houfan;He, Youzhou
首次成功制备了以单原子Pt嵌入PtII四（4-羧基苯基）卟啉（PtTCPP）为连接基团，ti -氧分子簇为金属节点的坚固高效钛金属有机骨架（TMF-Pt），并通过像差校正扫描透射电子显微镜（HAADF-STEM）和基于同步辐射的x射线吸收精细结构光谱（XAFS）进行了证实。并应用于光催化制氢和脱除NO。值得注意的是，与大多数已报道的mofs基光催化剂相比，TMF-Pt表现出极高的析氢活性（15456 mu mol.g- 1.h- 1）和NO去除率（70.3%），这可能归因于单原子Pt具有很高的原子利用效率和较高的载流子分离效率，以及Ti-oxo簇作为著名的TiO2光催化剂的替代品。结果为我们提供了一种新的策略，将单原子Pt引入卟啉骨架的中心，可以将广泛的光捕获卟啉与非常高的原子利用效率的单原子Pt结合起来，最终进一步提高光催化性能。
A robust and efficient titanium metal-organic framework (TMF-Pt) with a single-atom Pt embedded PtII tetrakis (4-carboxyphenyl)porphyrins (PtTCPP) as linking groups and Ti-oxo molecular clusters as metal nodes was successfully fabricated for the first time, which have been confirmed by aberration-correction scanning transmission electron microscopy (HAADF-STEM) and synchrotron-radiation-based X-ray absorption fine-structure spectroscopy (XAFS), and was applied to photocatalytic hydrogen production and NO removal. It was worth noting that the TMF-Pt exhibited an extremely high hydrogen evolution activity (15456 mu mol.g- 1.h- 1) and NO removal rate (70.3%) in comparison with most of the reported MOFs-based photocatalysts, which could be ascribed to the very high atom-utilization efficiency of single-atom Pt along with a high charge carriers separation efficiency and the Ti-oxo clusters as an alternative to the very famous TiO2 photocatalyst. The results provided us with a novel strategy that introducing single-atom Pt into the center of the porphyrin skeleton could integrate the broad light-harvesting porphyrin unite with the very high atom-utilization efficiency single-atom Pt to further improve the photocatalytic performance ultimately.