Journal
CHEMOSPHERE
Volume 287, Issue -, Pages -Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.chemosphere.2021.132293
Keywords
Air purification; Formaldehyde; Catalytic oxidation; Density functional theory
Categories
Funding
- Basic Science Center Project for National Natural Science Foundation of China [72088101]
- China Postdoctoral Science Foundation [2020T130730]
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Water plays a crucial role in the catalytic oxidation of formaldehyde by influencing the phase structure and morphology of birnessite. The presence of hydroxyl groups accelerates the oxidation reaction of formaldehyde and facilitates the formation of oxygen vacancies. The continuous decomposition of formaldehyde by birnessite is attributed to the favorable effect of water on the catalytic reaction.
Water is featured in an indispensable role during the process of catalytic oxidation of HCHO. In this work, a rich water-containing birnessite-type MnO2 was synthesized, and its water content was adjusted through calcination. Phase structure and texture properties of the prepared birnessite were characterized. It was revealed that three types of water (namely absorbed water, molecular water, and structural hydroxyl) existed in birnessite. With the loss of water content, the interlayer distance of samples had decreased which changed the structure of birnessite to cryptomelane. This converted the morphology from an initial layered shape to a rod-like shape. Besides, the underlying mechanism for this effect on HCHO catalytic oxidation was elucidated. Results indicated that hydroxyl groups could slowly and sequentially oxidize HCHO to DOM, formate, and carbonate species. The hydroxyl groups also promoted the formation of oxygen vacancy which could activate O2 to O- 2 and O- . The hydroxyl groups which were consumed had originally been supplied by the reaction between O- 2, O- , and H2O (absorbed and interlayer water in birnessite) which was then replenished from air stream. Clearly, water is favorable to the catalytic reaction. It is the main reason why birnessite can continuously decompose HCHO.
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