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基于钴卟啉的金属有机框架上高选择性光催化将 CO 转化为液态太阳能燃料

High selective photocatalytic CO conversion into liquid solar fuel over a cobalt porphyrin-based metal-organic framework.

作者信息

Sadeghi N, Sillanpää Mika

机构信息

Department of Chemical Engineering, Laval University, Quebec, G1V 0A8, Canada.

Environmental Engineering and Management Research Group, Ton Duc Thang University, Ho Chi Minh City, Vietnam.

出版信息

Photochem Photobiol Sci. 2021 Mar;20(3):391-399. doi: 10.1007/s43630-021-00027-9. Epub 2021 Mar 12.

Abstract

In the present study, porphyrin-based metal-organic framework (Co/PMOF) was synthesized and characterized by different spectra analyses. The photoluminescence properties of porphyrin and Co/PMOF revealed that the photoluminescence of Co/PMOF was quenched compared to the porphyrin, indicating that the lifetime of photo-generated charge carriers in Co/PMOF is longer than porphyrin. The prepared Co/PMOF was applied as an efficient photocatalyst for CO photoconversion to formate in the presence of triethanolamine (TEOA) as a sacrificial agent under visible-light irradiation. The photoreaction results showed that 23.21 µmol HCOO was produced over Co/PMOF during the 6 h photocatalytic reaction under visible illumination, showing much better activity than the porphyrin, 4.56 µmol HCOO. No other products were detected, suggesting that this reaction over Co/PMOF has high selectivity. Co/PMOF reusability and stability were examined through recycling tests and there were no remarkable losses of photoactivity even after three cycles of photoreaction. Moreover, FTIR measurement and UV-Vis spectra demonstrated no notable changes in Co/PMOF structure. As a result, superior photocatalytic behavior of Co/PMOF was implied for CO photoreduction which highlights the great potential of assembly porphyrin and cobalt into MOFs for CO photoreduction.

摘要

在本研究中,合成了基于卟啉的金属有机框架(Co/PMOF),并通过不同的光谱分析对其进行了表征。卟啉和Co/PMOF的光致发光特性表明,与卟啉相比,Co/PMOF的光致发光被猝灭,这表明Co/PMOF中光生载流子的寿命比卟啉长。制备的Co/PMOF在可见光照射下,以三乙醇胺(TEOA)作为牺牲剂,被用作将CO光催化转化为甲酸盐的高效光催化剂。光反应结果表明,在可见光照射下进行6小时的光催化反应过程中,Co/PMOF上产生了23.21 μmol的HCOO,其活性比卟啉(4.56 μmol HCOO)好得多。未检测到其他产物,这表明Co/PMOF上的该反应具有高选择性。通过循环测试考察了Co/PMOF的可重复使用性和稳定性,即使经过三个光反应循环,光活性也没有明显损失。此外,傅里叶变换红外光谱测量和紫外可见光谱表明Co/PMOF的结构没有明显变化。结果表明,Co/PMOF在CO光还原方面具有优异的光催化性能,这突出了将卟啉和钴组装到金属有机框架中用于CO光还原的巨大潜力。

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