• 文献标题:   Near-Infrared-Driven Selective Photocatalytic Removal of Ammonia Based on Valence Band Recognition of an alpha-MnO2/N-Doped Graphene Hybrid Catalyst
  • 文献类型:   Article
  • 作  者:   LIU WX, ZHU XL, LI SQ, GU QQ, MENG ZD
  • 作者关键词:  
  • 出版物名称:   ACS OMEGA
  • ISSN:   2470-1343
  • 通讯作者地址:   Suzhou Univ Sci Technol
  • 被引频次:   3
  • DOI:   10.1021/acsomega.8b00161
  • 出版年:   2018

▎ 摘  要

Near-infrared (NIR)-response photocatalysts are desired to make use of 44% NIR solar irradiation. A flower-like alpha-MnO2/N-doped graphene (NG) hybrid catalyst was synthesized and characterized by X-ray diffraction spectroscopy, transmission electron microscopy, Raman spectroscopy, UV-vis-NIR diffuse reflectance spectroscopy, and X-ray photoelectron spectroscopy. The flower-like material of alpha-MnO2/NG was oval-shaped with the semi major axis of 140 nm and semi minor axis of 95 nm and the petal thickness of 3.5-8.0 nm. The indirect band gap was measured to be 1.16 eV, which is very close to 0.909 eV estimated by the first-principles calculation. The band gap can harvest NIR irradiation to 1069 nm. The coupling of alpha-MnO2 with NG sheets to form alpha-MnO2/NG can significantly extend the spectrum response up to 1722 nm, improving dramatically the photocatalytic activity. The experimental results displayed that the alpha-MnO2/NG hybrid catalyst can recognize ammonia in methyl orange (MO)-ammonia, rhodamine B (RHB)-ammonia, and humic acid-ammonia mixed solutions and selectively degrade ammonia. The degradation ratio of ammonia reached over 93.0% upon NIR light irradiation in the mixed solutions, while those of MO, RHB, and humic acid were only 9.7, 9.4, and 15.7%, respectively. The products formed during the photocatalytic process were followed with ion chromatography, gas chromatography, and electrochemistry. The formed nitrogen gas has been identified during the photocatalytic process. A valence band recognition model was suggested based on the selective degradation of ammonia via alpha-MnO2/NG.