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High-performance of Cu-TiO2 for photocatalytic oxidation of formaldehyde under visible light and the mechanism study

机译:可见光下的甲醛的光催化氧化Cu-TiO2的高性能和机制研究

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摘要

Photocatalysis is regarded as a promising method for indoor formaldehyde (HCHO) removal, and there remains a strong demand for the development of highly efficient photocatalysts for HCHO oxidation under visible light. Herein, by grafting nano CuOx clusters onto TiO2, the higher performance is achieved over Cu-TiO2 for the photocatalytic oxidation of HCHO under visible light compared with the typical photocatalysts N-TiO2 and g-C3N4. It is found that the presence of water greatly promotes the activity of HCHO oxidation on Cu-TiO2. The characterization results indicate that the CuOx clusters on TiO2 exhibit high redox reversibility between Cu (II) and Cu (I) and greatly facilitate the migration of electrons. The mechanism of photocatalytic oxidation of HCHO was explored by using in situ DRIFTS measurements and DFT calculations. It is shown that HCHO is firstly oxidized to dioxymethylene (DOM), and then DOM is transformed into formate species under visible light irradiation. DFT calculations results indicate that the (OH)-O-center dot species are responsible for surface formate decomposition, which is the rate-determining step, while O-center dot(2)- radical is not active in formate decomposition. Our findings improve the understanding on the photocatalytic oxidation of HCHO, and the Cu-TiO2 catalyst is a promising candidate for practical application in indoor air purification.
机译:光催化被认为是用于室内甲醛(HCHO)去除的有希望的方法,并且仍然对在可见光下对HCHO氧化的高效光催化剂的开发的强烈需求。这里,通过将纳米CuOx簇移植到TiO 2上,与典型的光催化剂N-TiO2和G-C3N4相比,通过Cu-TiO 2通过Cu-TiO 2实现高度的性能,用于在可见光下的可见光下的光催化氧化。发现水的存在大大促进了在Cu-TiO 2上促进了Hcho氧化的活性。表征结果表明,TiO 2上的Cuox簇在Cu(II)和Cu(I)之间表现出高氧化还原可逆性,并且极大地促进了电子的迁移。通过使用原位漂移测量和DFT计算,探索了Hcho的光催化氧化机制。结果表明,首先将Hcho氧化成二氧二甲基(DOM),然后在可见光照射下转化为甲酸物种。 DFT计算结果表明(OH)-O-中心点物种负责表面甲酸分解,这是速率确定步骤,而O-Center Dot(2) - 自由基在甲酸分解中不活跃。我们的研究结果改善了对Hcho光催化氧化的理解,Cu-TiO2催化剂是室内空气净化中的实际应用的有希望的候选者。

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