4.8 Article

Surface Lattice Oxygen Activation by Nitrogen-Doped Manganese Dioxide as an Effective and Longevous Catalyst for Indoor HCHO Decomposition

期刊

ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 23, 页码 26960-26970

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c04369

关键词

nitrogen-doping; catalytic oxidation; lattice oxygen; HCHO removal; room temperature

资金

  1. Provincial Nature Science Foundation of Sichuan [2017CC0017, 2018FZ0105, 2019YJ0025]
  2. National Key R&D Program of China [2018YFB1502700]
  3. Research and Development Program of Chengdu [2019-YF05-01193-SN]

向作者/读者索取更多资源

The thermodynamic stability of oxygen vacancy in catalytic oxidation of formaldehyde can be improved by nitrogen doping, leading to enhanced catalytic activity and stability of MnO2/C catalyst for HCHO oxidation. The nitrogen-doped MnO2/C catalyst can completely remove around 1 ppm of HCHO within 3 hours and remains highly active even after 5 cycles at room temperature, showing great potential for application in the field of HCHO oxidation.
Oxygen vacancy plays an important role in catalytic oxidation of formaldehyde (HCHO), but the inherent drawback of its thermodynamic instability causes the deactivation of catalysts. Hence, improving the thermodynamic stability of oxygen vacancy is a crux during HCHO oxidation. Here, a novel and simple nitrogen doping of MnO2/C catalyst is designed for HCHO oxidation at room temperature. The surface lattice oxygen of MnO2 will be activated by nitrogen-doping, which acts as active sites for HCHO oxidation and solves the thermodynamic instability issue of oxygen vacancy. Furthermore, carbon is doped with nitrogen to promote electron transfer and accelerate the HCHO oxidation process. Therefore, the catalytic activity and stability of the catalyst can be significantly promoted, which can completely remove similar to 1 ppm HCHO in the tank within 3 h, and remains highly active after 5 cycles at room temperature (RH = 55%). In addition, the excellent removal performance over the prepared catalyst is also attributed to abundant surface oxygen species, amorphous crystallinity, and low reduction temperature. In situ diffuse reflectance infrared Fourier transform spectrometry (DRIFTS) and density functional theory (DFT) calculations reveal the reaction mechanism of HCHO. This strategy provides crucial enlightenment for designing novel Mn-based catalysts for application in the HCHO oxidation field.

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