3D Lanthanide Neodymium Porphyrin Metal–Organic Framework for Photocatalytic Oxidation of Styrene,Inorganic Chemistry

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3D Lanthanide Neodymium Porphyrin Metal–Organic Framework for Photocatalytic Oxidation of Styrene
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2023-05-16 , DOI: 10.1021/acs.inorgchem.3c00827
Yuxuan Qi ₁ , Chenglong Zheng ₁ , Zhiquan Cai ₁ , Zhifei Cheng ₂ , Tinghao Yu ₁ , Xiao-Xuan Li ₁ , Shilu Fan _{1,

3} , Yi-Si Feng _{1,

3}

Affiliation

A novel three-dimensional lanthanide porphyrin-based MOF (Nd-PMOFs) was synthesized by using tetracarboxyphenyl porphyrin as the ligand and the lanthanide Nd as the coordination metal. Its specific crystal structure information was obtained by single-crystal diffraction with the space group C2/c and the empirical formula C₇₂H₄₅N₆Nd₂O_15.25. This new Nd porphyrin-based MOF with an organic framework formed by a unique coordination method enables the effective separation of photogenerated electrons and holes under photoluminescence, giving it excellent photocatalytic property which could be verified by the characterization data. The photocatalytic performance was examined by taking tert-butyl hydroperoxide as the oxidant and Nd-PMOFs as the catalyst for photocatalytic oxidation of styrene to benzaldehyde with 91.4% conversion and 81.2% benzaldehyde selectivity under optimal reactions, which surpasses most of the results reported in the literature. Several styrenes with other substituents were screened to explore the general applicability of Nd-PMOF for photocatalysis of styrene, among which Nd-PMOFs also exhibited excellent photocatalytic performance. This work offers the possibility to apply lanthanide organometallic frameworks, which are widely used in fluorescent materials, to photocatalysis. In addition, it also provides a new method for the catalytic generation of benzaldehyde from styrene that is consistent with the needs of modern green development.

中文翻译：

用于苯乙烯光催化氧化的 3D 镧系元素卟啉金属-有机骨架

以四羧基苯基卟啉为配体，镧系元素Nd为配位金属，合成了一种新型三维镧系卟啉基MOFs（Nd-PMOFs）。其具体晶体结构信息通过单晶衍射获得，空间群为C 2 / c，经验式为C ₇₂ H ₄₅ N ₆ Nd ₂ O _15.25. 这种新型 Nd 卟啉基 MOF 具有通过独特的配位方法形成的有机骨架，能够在光致发光下有效分离光生电子和空穴，使其具有优异的光催化性能，可通过表征数据进行验证。光催化性能通过采取叔-丁基氢过氧化物作为氧化剂和 Nd-PMOFs 作为催化剂光催化氧化苯乙烯制苯甲醛，在最佳反应下转化率为 91.4%，苯甲醛选择性为 81.2%，超过了大多数文献报道的结果。筛选了几种具有其他取代基的苯乙烯，以探索 Nd-PMOF 在苯乙烯光催化中的普遍适用性，其中 Nd-PMOF 还表现出优异的光催化性能。这项工作为将广泛用于荧光材料的镧系元素有机金属框架应用于光催化提供了可能性。此外，还为苯乙烯催化生成苯甲醛提供了一种符合现代绿色发展需要的新方法。

更新日期：2023-05-16

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