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Highly selective photocatalytic oxidation of 5-hydroxymethylfurfural by interfacial Pt–O bonding Pt–Ov–BiOBr
New Journal of Chemistry ( IF 3.3 ) Pub Date : 2023-02-28 , DOI: 10.1039/d3nj00498h
Ming Gong 1 , Hui Zhao 1 , Chengsi Pan 1 , Yuming Dong 1 , Yingxin Guo 1 , Haixia Li 1 , Jiawei Zhang 1 , Guangli Wang 1 , Yongfa Zhu 2
Affiliation  

The photocatalytic oxidation of 5-hydroxymethylfurfural (HMF) has the advantages of mild conditions and a controllable oxidation degree. There are a number of methods to increase its reactivity by boosting the production of ˙O2, among which using metal-modified semiconductor catalyst systems is one of the most promising methods. Although several metal-modified semiconductor catalyst systems have been successfully designed, only a small number of them have been used in photocatalytic selective oxidation, and the contact interface between the metal and semiconductor catalysts has not been well studied. Here, interfacial Pt–O bonded Pt–Ov–BiOBr catalysts were designed for photocatalytic HMF selective oxidation. Due to the environment of unsaturated coordination on Ov–BiOBr, Pt can form a Pt–O bond as an electron transport channel to transfer photogenerated electrons from Ov–BiOBr to Pt for efficient generation of ˙O2. Meanwhile, photogenerated h+ will gather at the interface between Pt and Ov–BiOBr contact to oxidize HMF to carbon-centered radicals. The spatial proximity of the ˙O2 and carbon-centered radicals at the Pt–Ov–BiOBr contact interface promotes reciprocal collisions and consequently reactions. Additionally, Pt–Ov–BiOBr was found to have excellent photogenerated electron–hole separation efficiency by photoelectric characterization, and the ESR and O2-TPD results showed that Pt can activate oxygen more effectively to produce ˙O2. As a result, the conversion rate of HMF selective oxidation of Pt–Ov–BiOBr becomes 4.6 times higher and the selectivity becomes 2.2 times higher compared to those of BiOBr. This study suggests that an appropriately designed metal–semiconductor contact interface can boost the effectiveness of HMF photocatalytic selective oxidation.

中文翻译:

界面 Pt-O 键合 Pt-Ov-BiOBr 高选择性光催化氧化 5-羟甲基糠醛

5-羟甲基糠醛(HMF)的光催化氧化具有条件温和、氧化程度可控等优点。有多种方法可以通过促进 ˙O 2的产生来提高其反应性-,其中使用金属修饰的半导体催化剂体系是最有前途的方法之一。尽管已经成功设计了几种金属修饰的半导体催化剂体系,但只有少数用于光催化选择性氧化,金属与半导体催化剂之间的接触界面还没有得到很好的研究。在这里,界面 Pt-O 键合 Pt-Ov-BiOBr 催化剂被设计用于光催化 HMF 选择性氧化。由于Ov-BiOBr 上的不饱和配位环境,Pt 可以形成Pt-O 键作为电子传输通道,将光生电子从Ov-BiOBr 转移到Pt,从而有效生成˙O 2 。同时,光生 h +将聚集在 Pt 和 Ov-BiOBr 接触之间的界面,将 HMF 氧化成以碳为中心的自由基。Pt-Ov-BiOBr 接触界面处的˙O 2 −和以碳为中心的自由基在空间上的接近促进了相互碰撞和随后的反应。此外,通过光电表征发现Pt-Ov-BiOBr具有优异的光生电子-空穴分离效率,ESR和O 2 -TPD结果表明Pt可以更有效地激活氧产生˙O 2 . 因此,与 BiOBr 相比,HMF 选择性氧化 Pt-Ov-BiOBr 的转化率提高了 4.6 倍,选择性提高了 2.2 倍。这项研究表明,适当设计的金属-半导体接触界面可以提高 HMF 光催化选择性氧化的有效性。
更新日期:2023-02-28
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