Room-Temperature Oxidation of Formaldehyde by Layered Manganese Oxide: Effect of Water

双锰矿 高锰酸钾 化学 吸附 无机化学 甲醛 高锰酸盐 氧化剂 草酸盐 解吸 碳酸盐 煅烧 催化作用 有机化学 氧化锰
作者
Jinlong Wang,Pengyi Zhang,Jinge Li,Chuanjia Jiang,Rizwangul Yunus,Jeong-Hyun Kim
出处
期刊:Environmental Science & Technology [American Chemical Society]
卷期号:49 (20): 12372-12379 被引量:376
标识
DOI:10.1021/acs.est.5b02085
摘要

Layered manganese oxide, i.e., birnessite was prepared via the reaction of potassium permanganate with ammonium oxalate. The water content in the birnessite was adjusted by drying/calcining the samples at various temperatures (30 °C, 100 °C, 200 °C, 300 °C, and 500 °C). Thermogravimetry-mass spectroscopy showed three types of water released from birnessite, which can be ascribed to physically adsorbed H2O, interlayer H2O and hydroxyl, respectively. The activity of birnessite for formaldehyde oxidation was positively associated with its water content, i.e., the higher the water content, the better activity it has. In-situ DRIFTS and step scanning XRD analysis indicate that adsorbed formaldehyde, which is promoted by bonded water via hydrogen bonding, is transformed into formate and carbonate with the consumption of hydroxyl and bonded water. Both bonded water and water in air can compensate the consumed hydroxyl groups to sustain the mineralization of formaldehyde at room temperature. In addition, water in air stimulates the desorption of carbonate via water competitive adsorption, and accordingly the birnessite recovers its activity. This investigation elucidated the role of water in oxidizing formaldehyde by layered manganese oxides at room temperature, which may be helpful for the development of more efficient materials.
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