甲醛在tio2和pt纳米团簇表面解离吸附和脱氢氧化-dissociative adsorption and dehydrooxidation of formaldehyde on tio _ 2 and pt nanoclusters.docxVIP

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甲醛在tio2和pt纳米团簇表面解离吸附和脱氢氧化-dissociative adsorption and dehydrooxidation of formaldehyde on tio _ 2 and pt nanoclusters.docx

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甲醛在tio2和pt纳米团簇表面解离吸附和脱氢氧化-dissociative adsorption and dehydrooxidation of formaldehyde on tio _ 2 and pt nanoclusters

AbstractFormaldehyde (HCHO), a colorless and pungent-smelling gas, is considered as the main indoor air pollutant in modern houses, which easily combines with proteins in the human body and increases the risks of some diseases including cancer. Thus many methods, such as adsorption and oxidation, are used to remove HCHO from air. However, in practical application, the adsorption and oxidation of HCHO both suffer from some limitations, such as poor renewability, high cost and low efficiency. The investigation on mechanisms of HCHO adsorption and oxidation can provide the theoretical foundation for the future developments of HCHO adsorbent and catalyst. TiO2 is known for its strong chemical stability, no toxicity, rich source and low cost, which has been widely used in the purification of indoor air. Hence, the present paper is mainly focused on the mechanisms of HCHO adsorption and oxidation on anatase TiO2 surface. Those key factors influencing HCHO adsorption and oxidation are discussed in detail.The F?, OH? and Cl?-modified anatase TiO2 nanosheets (TNS) with exposed{001} facets were prepared by a simple hydrothermal and post-treatment method, and their HCHO adsorption performance and mechanism were investigated by the experimental analysis and theoretical simulations. Our results indicated that the adsorbed F?, OH? and Cl? ions all could weaken the interaction between HCHO and TNS surface, leading to the serious reduction of HCHO adsorption performance of TNS. However, different from F? and Cl? ions, OH? ion could induce the dissociative adsorption of HCHO by capturing one H atom from HCHO, resulting in the formation of one formyl group and one H2O-like group. This greatly reduced thetotal energy of HCHO adsorption system. Thus, the adsorbed OH? ions couldprovide the additional active centers for HCHO adsorption. As a result, the NaOH-treated TNS showed the best HCHO adsorption performance mainly because its surface F? was replaced OH?. This study will