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Fe Doped MIL-101/Graphene Nanohybrid for Photocatalytic Oxidation of Alcohols Under Visible-Light Irradiation
Catalysis Letters ( IF 2.3 ) Pub Date : 2021-01-02 , DOI: 10.1007/s10562-020-03472-w
Mingming Wang , Yali Ma , Bolin Lv , Fenglin Hua , Shuangyan Meng , Xuedi Lei , Qingtao Wang , Bitao Su , Ziqiang Lei , Zhiwang Yang

A novel photoactive porous material of GR/FeMIL-101 based on FeMIL-101 metal organic frameworks (MOFs) was successfully synthesized via a simple hydrothermal method. The structural and photoelectric properties of the GR/FeMIL-101 was analyzed by XRD, SEM, TEM, TGA, XPS, UV–vis DRS, FT-IR, PL and EIS methods. The photocatalytic performance for the selective oxidation of benzyl alcohol with GR/FeMIL-101 as catalysts was evaluated under visible light irradiation. The results showed that the GR/FeMIL-101 nanohybrid had better photocatalytic performance than both of FeMIL-101 and the pristine MIL-101. It was further found that the incorporation of Fe and MIL-101 caused valence fluctuations of Fe3+/Fe2+ which improved the absorption of visible-light and increased the separation efficiency of photogenerated charges. In addition, the combination of FeMIL-101 and GR could further promote the transfer rate of the photoelectrons. The mechanism of the reaction revealed that ·O2− was the dominating active specie in this reaction through active species trapping experiments. Fe doped MIL-101/GR nanohybrid was successfully synthesized as an efficient photocatalyst for selective oxidation of alcohols under visible-light and shown a best conversion of 50%. Analyses revealed that Fe was successfully doped into the MIL-101, valence fluctuation of Fe2+/Fe3+ not only improved the visible-light absorption but also increased the separation rate of photoexcited carriers. Graphene further improved the transportation rate of electron (e-). Subsequently, the possible photocatalytic mechanism for the selective oxidation of alcohols was proposed. It was proved that superoxide radicals (·O2-) was the main active species when the reaction was performed under Oxygen atmosphere.

中文翻译:

Fe掺杂的MIL-101/石墨烯纳米杂化物用于可见光照射下醇的光催化氧化

通过简单的水热法成功合成了一种基于 FeMIL-101 金属有机骨架 (MOF) 的新型 GR/FeMIL-101 光活性多孔材料。通过XRD、SEM、TEM、TGA、XPS、UV-vis DRS、FT-IR、PL和EIS方法分析了GR/FeMIL-101的结构和光电性能。在可见光照射下评估了以GR/FeMIL-101为催化剂选择性氧化苯甲醇的光催化性能。结果表明,GR/FeMIL-101 纳米杂化物比 FeMIL-101 和原始 MIL-101 具有更好的光催化性能。进一步发现Fe和MIL-101的掺入引起Fe3+/Fe2+的价态波动,从而改善了可见光的吸收并提高了光生电荷的分离效率。此外,FeMIL-101 和 GR 的结合可以进一步提高光电子的传输速率。反应机理通过活性物种捕获实验揭示了·O2-是该反应中的主要活性物种。Fe掺杂的MIL-101/GR纳米杂化物被成功合成为一种在可见光下选择性氧化醇的有效光催化剂,并显示出50%的最佳转化率。分析表明,Fe成功掺杂到MIL-101中,Fe2+/Fe3+的价态波动不仅提高了可见光吸收,而且提高了光激发载流子的分离率。石墨烯进一步提高了电子(e-)的传输速率。随后,提出了醇类选择性氧化可能的光催化机理。
更新日期:2021-01-02
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