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

机译:层状氧化锰在室温下氧化甲醛:水的影响

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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 ℃, 100 ℃, 200 ℃, 300 ℃, and 500 ℃). Thermogravimetry-mass spectroscopy showed three types of water released from birnessite, which can be ascribed to physically adsorbed H_2O, interlayer H_2O 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.
机译:通过高锰酸钾与草酸铵的反应制备层状氧化锰,即水钠锰矿。通过在各种温度(30℃,100℃,200℃,300℃和500℃)下干燥/煅烧样品来调整水钠锰矿中的水含量。热重-质谱法显示从水钠锰矿中释放出三种类型的水,分别归因于物理吸附的H_2O,层间H_2O和羟基。水钠锰矿对甲醛氧化的活性与其水含量呈正相关,即水含量越高,其活性越好。原位DRIFTS和X射线扫描XRD分析表明,吸附的甲醛(通过氢键结合的水促进了甲醛的吸附)被羟基和键合水的消耗转化为甲酸盐和碳酸盐。结合水和空气中的水都可以补偿消耗的羟基,以维持室温下甲醛的矿化。另外,空气中的水通过水竞争性吸附刺激碳酸盐的解吸,因此水钠锰矿恢复其活性。这项研究阐明了水在室温下通过层状锰氧化物氧化甲醛的作用,这可能有助于开发更有效的材料。

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  • 来源
    《Environmental Science & Technology》 |2015年第20期|12372-12379|共8页
  • 作者单位

    State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China,Collaborative Innovation Center for Regional Environmental Quality, School of Environment, Tsinghua University, Beijing 100084, China;

    State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China,Collaborative Innovation Center for Regional Environmental Quality, School of Environment, Tsinghua University, Beijing 100084, China;

    State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China;

    Department of Civil and Environmental Engineering, Duke University, Durham, North Carolina 90287, United States;

    State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China;

    State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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