Tremendous Effect of the Morphology of Birnessite-Type Manganese Oxide Nanostructures on Catalytic Activity

被引:188
作者
Hou, Jingtao [1 ]
Li, Yuanzhi [1 ]
Mao, Mingyang [1 ]
Ren, Lu [1 ]
Zhao, Xiujian [1 ]
机构
[1] Wuhan Univ Technol, State Key Lab Silicate Mat Architectures, Wuhan 430070, Peoples R China
基金
中国国家自然科学基金;
关键词
catalytic; manganese oxide; morphology effect; oxygen vacancy; VOLATILE ORGANIC-COMPOUNDS; INITIO MOLECULAR-DYNAMICS; WATER-OXIDATION CATALYSIS; SIGNIFICANT ENHANCEMENT; LAYERED MNO2; BENZENE; DECOMPOSITION; REMOVAL; OXYGEN; OMS-2;
D O I
10.1021/am5027743
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
The octahedral layered birnessite-type manganese oxide (OL-1) with the morphologies of nanoflowers, nanowires, and nanosheets were prepared and characterized with X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), thermogravimetric/differential scanning calorimetry (TG/DSC), Brunnauer-Emmett-Teller (BET), inductively coupled plasma (ICP), and X-ray photoelectron spectroscopy (XPS). The OL-1 nanoflowers possess the highest concentration of oxygen vacancies or Mn3+, followed by the OL-1 nanowires and nanosheets. The result of catalytic tests shows that the OL-1 nanoflowers exhibit a tremendous enhancement in the catalytic activity for benzene oxidation as compared to the OL-1 nanowires and nanosheets. Compared to the OL-1 nanosheets, the OL-1 nanoflowers demonstrate an enormous decrease (Delta T-50 = 274 degrees C; Delta T-90 > 248 degrees C) in reaction temperatures T-50 and T-90 (corresponding to 50 and 90% benzene conversion, respectively) for benzene oxidation. The origin of the tremendous effect of morphology on the catalytic activity for the nanostructured OL-1 catalysts is experimentally and theoretically studied via CO temperature-programmed reduction (CO-TPR) and density functional theory (DFT) calculation. The tremendous catalytic enhancement of the OL-1 nanoflowers compared to the OL-1 nanowires and nanosheets is attributed to their highest surface area as well as their highest lattice oxygen reactivity due to their higher concentration of oxygen vacancies or Mn3+, thus tremendously improving the catalytic activity for the benzene oxidation.
引用
收藏
页码:14981 / 14987
页数:7
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